Metabolism of americium-241 in dairy animals. [Cows and goats

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sutton, W.W.; Patzer, R.G.; Mullen, A.A.

1978-10-01

Groups of lactating cows and goats were used to examine americium-241 metabolism in dairy animals. Following either single oral or intravenous nuclide doses, samples of milk, urine, blood, and feces were taken over a 168-hr collection period and the americium concentrations were determined by gamma counting. Gastrointestinal uptake of americium by both cows and goats was estimated to be 0.014% of the respective oral doses. The cumulative percentage of oral dose transported to milk and urine was 4.4 x 10/sup -4/ and 1.1 x 10/sup -3/ respectively for cows and 4.4 x 10/sup -3/ and 1.2 x 10/sup -3/ respectivelymore » for goats. The relatively high americium concentrations noted in caprine milk following the oral doses are discussed. Plasma concentrations of americium decreased rapidly following all intravenous injections. The average percentage of injected americium transferred to milk, urine, and feces was 3, 6, and 2% respectively for cows and 2, 4, and 2% respectively for goats. In both intravenously dosed groups, approximately 30% of all americium released from the body was found in the urine during the first 24 hrs after injection. All animals were sacrificed 8 to 9 days after dosing. Bovine bone retained the greatest fraction of the administered dose followed by the liver. However, liver retained the greatest amount of americium in the goats following both oral and intravenous doses. Comparisons are presented between americium-241 and plutonium-238 transport in dairy cows.« less

Thermodynamic and Spectroscopic Studies of Trivalent f -element Complexation with Ethylenediamine- N,N '-di(acetylglycine)- N,N '-diacetic Acid

DOE Office of Scientific and Technical Information (OSTI.GOV)

Heathman, Colt R.; Grimes, Travis S.; Zalupski, Peter R.

In this study, the coordination behavior and thermodynamic features of complexation of trivalent lanthanides and americium by ethylenediamine- N,N'-di(acetylglycine)- N,N'-diacetic acid (EDDAG-DA) (bisamide-substituted-EDTA) were investigated by potentiometric and spectroscopic techniques. Acid dissociation constants (K a) and complexation constants (β) of lanthanides (except Pm) were determined by potentiometric analysis. Absorption spectroscopy was used to determine stability constants for the binding of trivalent americium and neodymium by EDDAG-DA under similar conditions. The potentiometry revealed 5 discernible protonation constants and 3 distinct metal–ligand complexes (identified as ML –, MHL, and MH 2L +). Time-resolved fluorescence studies of Eu-(EDDAG-DA) solutions (at varying pH) identifiedmore » a constant inner-sphere hydration number of 3, suggesting that glycine functionalities contained in the amide pendant arms are not involved in metal complexation and are protonated under more acidic conditions. The thermodynamic studies identified that f-element coordination by EDDAG-DA is similar to that observed for ethylenediamine- N,N,N',N'-tetraacetic acid (EDTA). However, coordination via two amidic oxygens of EDDAG-DA lowers its trivalent f-element complex stability by roughly 3 orders of magnitude relative to EDTA.« less

Thermodynamic and Spectroscopic Studies of Trivalent f -element Complexation with Ethylenediamine- N,N '-di(acetylglycine)- N,N '-diacetic Acid

DOE PAGES

Heathman, Colt R.; Grimes, Travis S.; Zalupski, Peter R.

2016-03-21

In this study, the coordination behavior and thermodynamic features of complexation of trivalent lanthanides and americium by ethylenediamine- N,N'-di(acetylglycine)- N,N'-diacetic acid (EDDAG-DA) (bisamide-substituted-EDTA) were investigated by potentiometric and spectroscopic techniques. Acid dissociation constants (K a) and complexation constants (β) of lanthanides (except Pm) were determined by potentiometric analysis. Absorption spectroscopy was used to determine stability constants for the binding of trivalent americium and neodymium by EDDAG-DA under similar conditions. The potentiometry revealed 5 discernible protonation constants and 3 distinct metal–ligand complexes (identified as ML –, MHL, and MH 2L +). Time-resolved fluorescence studies of Eu-(EDDAG-DA) solutions (at varying pH) identifiedmore » a constant inner-sphere hydration number of 3, suggesting that glycine functionalities contained in the amide pendant arms are not involved in metal complexation and are protonated under more acidic conditions. The thermodynamic studies identified that f-element coordination by EDDAG-DA is similar to that observed for ethylenediamine- N,N,N',N'-tetraacetic acid (EDTA). However, coordination via two amidic oxygens of EDDAG-DA lowers its trivalent f-element complex stability by roughly 3 orders of magnitude relative to EDTA.« less

Supported liquid inorganic membranes for nuclear waste separation

DOEpatents

Bhave, Ramesh R; DeBusk, Melanie M; DelCul, Guillermo D; Delmau, Laetitia H; Narula, Chaitanya K

2015-04-07

A system and method for the extraction of americium from radioactive waste solutions. The method includes the transfer of highly oxidized americium from an acidic aqueous feed solution through an immobilized liquid membrane to an organic receiving solvent, for example tributyl phosphate. The immobilized liquid membrane includes porous support and separating layers loaded with tributyl phosphate. The extracted solution is subsequently stripped of americium and recycled at the immobilized liquid membrane as neat tributyl phosphate for the continuous extraction of americium. The sequestered americium can be used as a nuclear fuel, a nuclear fuel component or a radiation source, and the remaining constituent elements in the aqueous feed solution can be stored in glassified waste forms substantially free of americium.

Intramolecular sensitization of americium luminescence in solution: Shining light on short-lived forbidden 5f transitions

DOE PAGES

Sturzbecher-Hoehne, M.; Yang, P.; D'Aleo, A.; ...

2016-03-10

In this study, the photophysical properties and solution thermodynamics of water soluble trivalent americium (Am III) complexes formed with multidentate chromophore-bearing ligands, 3,4,3-LI(1,2-HOPO), Enterobactin, and 5-LIO(Me-3,2-HOPO), were investigated. The three chelators were shown to act as antenna chromophores for AmIII, generating sensitized luminescence emission from the metal upon complexation, with very short lifetimes ranging from 33 to 42 ns and low luminescence quantum yields (10 –3 to 10 –2%), characteristic of Near Infra-Red emitters in similar systems. The specific emission peak of Am III assigned to the 5D 1 → 7F 1 f–f transition was exploited to characterize the highmore » proton-independent stability of the complex formed with the most efficient sensitizer 3,4,3-LI(1,2-HOPO), with a log β 110 = 20.4 ± 0.2 value. In addition, the optical and solution thermodynamic features of these Am III complexes, combined with density functional theory calculations, were used to probe the influence of electronic structure on coordination properties across the f-element series and to gain insight into ligand field effects.« less

Intramolecular sensitization of americium luminescence in solution: shining light on short-lived forbidden 5f transitions

DOE PAGES

Sturzbecher-Hoehne, M.; Yang, P.; D'Aleo, A.; ...

2016-03-10

In this study, the photophysical properties and solution thermodynamics of water soluble trivalent americium (Am III) complexes formed with multidentate chromophore-bearing ligands, 3,4,3-LI(1,2-HOPO), Enterobactin, and 5-LIO(Me-3,2-HOPO), were investigated. The three chelators were shown to act as antenna chromophores for Am III, generating sensitized luminescence emission from the metal upon complexation, with very short lifetimes ranging from 33 to 42 ns and low luminescence quantum yields (10 -3 to 10 -2%), characteristic of Near Infra-Red emitters in similar systems. The specific emission peak of AmIII assigned to the 5D 1 → 7F 1 f–f transition was exploited to characterize the highmore » proton-independent stability of the complex formed with the most efficient sensitizer 3,4,3-LI(1,2-HOPO), with a log β 110 = 20.4 ± 0.2 value. In addition, the optical and solution thermodynamic features of these Am III complexes, combined with density functional theory calculations, were used to probe the influence of electronic structure on coordination properties across the f-element series and to gain insight into ligand field effects.« less

Electrochemical oxidation of 243Am(III) in nitric acid by a terpyridyl-derivatized electrode

DOE Office of Scientific and Technical Information (OSTI.GOV)

Dares, C. J.; Lapides, A. M.; Mincher, B. J.

A high surface area, tin-doped indium oxide electrode surface-derivatized with a terpyridine ligand has been applied to the oxidation of trivalent americium to Am(V) and Am(VI) in nitric acid. Potentials as low as 1.8 V vs. the saturated calomel electrode are used, 0.7 V lower than the 2.6 V potential for one-electron oxidation of Am(III) to Am(IV) in 1 M acid. This simple electrochemical procedure provides, for the first time, a method for accessing the higher oxidation states of Am in non-complexing media for developing the coordination chemistries of Am(V) and Am(VI) and, more importantly, for separation of americium frommore » nuclear waste streams.« less

Plutonium and americium separation from salts

DOEpatents

Hagan, Paul G.; Miner, Frend J.

1976-01-01

Salts or materials containing plutonium and americium are dissolved in hydrochloric acid, heated, and contacted with an alkali metal carbonate solution to precipitate plutonium and americium carbonates which are thereafter readily separable from the solution.

10 CFR 31.8 - Americium-241 and radium-226 in the form of calibration or reference sources.

Code of Federal Regulations, 2012 CFR

2012-01-01

... 10 Energy 1 2012-01-01 2012-01-01 false Americium-241 and radium-226 in the form of calibration or... BYPRODUCT MATERIAL § 31.8 Americium-241 and radium-226 in the form of calibration or reference sources. (a..., americium-241 or radium-226 in the form of calibration or reference sources: (1) Any person in a non...

10 CFR 31.8 - Americium-241 and radium-226 in the form of calibration or reference sources.

Code of Federal Regulations, 2014 CFR

2014-01-01

... 10 Energy 1 2014-01-01 2014-01-01 false Americium-241 and radium-226 in the form of calibration or... BYPRODUCT MATERIAL § 31.8 Americium-241 and radium-226 in the form of calibration or reference sources. (a..., americium-241 or radium-226 in the form of calibration or reference sources: (1) Any person in a non...

10 CFR 31.8 - Americium-241 and radium-226 in the form of calibration or reference sources.

Code of Federal Regulations, 2011 CFR

2011-01-01

... 10 Energy 1 2011-01-01 2011-01-01 false Americium-241 and radium-226 in the form of calibration or... BYPRODUCT MATERIAL § 31.8 Americium-241 and radium-226 in the form of calibration or reference sources. (a..., americium-241 or radium-226 in the form of calibration or reference sources: (1) Any person in a non...

10 CFR 31.8 - Americium-241 and radium-226 in the form of calibration or reference sources.

Code of Federal Regulations, 2010 CFR

2010-01-01

... 10 Energy 1 2010-01-01 2010-01-01 false Americium-241 and radium-226 in the form of calibration or... BYPRODUCT MATERIAL § 31.8 Americium-241 and radium-226 in the form of calibration or reference sources. (a..., americium-241 or radium-226 in the form of calibration or reference sources: (1) Any person in a non...

10 CFR 31.8 - Americium-241 and radium-226 in the form of calibration or reference sources.

Code of Federal Regulations, 2013 CFR

2013-01-01

... 10 Energy 1 2013-01-01 2013-01-01 false Americium-241 and radium-226 in the form of calibration or... BYPRODUCT MATERIAL § 31.8 Americium-241 and radium-226 in the form of calibration or reference sources. (a..., americium-241 or radium-226 in the form of calibration or reference sources: (1) Any person in a non...

Emergence of californium as the second transitional element in the actinide series

DOE PAGES

Cary, Samantha K.; Vasiliu, Monica; Baumbach, Ryan E.; ...

2015-04-16

A break in periodicity occurs in the actinide series between plutonium and americium as the result of the localization of 5f electrons. The subsequent chemistry of later actinides is thought to closely parallel lanthanides in that bonding is expected to be ionic and complexation should not substantially alter the electronic structure of the metal ions. Here we demonstrate that ligation of californium(III) by a pyridine derivative results in significant deviations in the properties of the resultant complex with respect to that predicted for the free ion. We expand on this by characterizing the americium and curium analogues for comparison, andmore » show that these pronounced effects result from a second transition in periodicity in the actinide series that occurs, in part, because of the stabilization of the divalent oxidation state. As a result, the metastability of californium(II) is responsible for many of the unusual properties of californium including the green photoluminescence.« less

Solvent Extraction Separation of Trivalent Americium from Curium and the Lanthanides

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jensen, Mark P.; Chiarizia, Renato; Ulicki, Joseph S.

2015-02-27

The sterically constrained, macrocyclic, aqueous soluble ligand N,N'-bis[(6-carboxy-2-pyridyl)methyl]-1,10-diaza-18-crown-6 (H2BP18C6) was investigated for separating americium from curium and all the lanthanides by solvent extraction. Pairing H2BP18C6, which favors complexation of larger f-element cations, with acidic organophosphorus extractants that favor extraction of smaller f-element cations, such as bis-(2-ethylhexyl)phosphoric acid (HDEHP) or (2-ethylhexyl)phosphonic acid mono(2-ethylhexyl) ester (HEH[EHP]), created solvent extraction systems with good Cm/Am selectivity, excellent trans-lanthanide selectivity (Kex,Lu/Kex,La = 108), but poor selectivity for Am against the lightest lanthanides. However, using an organic phase containing both a neutral extractant, N,N,N’,N’-tetra(2-ethylhexyl)diglycolamide (TEHDGA), and HEH[EHP] enabled rejection of the lightest lanthanides during loading ofmore » the organic phase from aqueous nitric acid, eliminating their interference in the americium stripping stages. In addition, although it is a macrocyclic ligand, H2BP18C6 does not significantly impede the mass transfer kinetics of the HDEHP solvent extraction system« less

Production and recovery of Americium-241

DOE Office of Scientific and Technical Information (OSTI.GOV)

Navratil, J.D.

1984-01-01

Americium-241, one of the most useful actinide isotopes, is produced as a by-product of plutonium scrap recovery operations. Rocky Flats (RF) has supplied high-purity americium oxide to the US Department of Energy's Isotope Pool since 1962. Over the years, the evolving separation and purification processes have included such diverse operations as aqueous precipitation, ion exchange, and both molten-salt and organic-solvent extraction. A review is presented of the production and recovery processes of americium-241. 5 references.

Postinhalation kinetics of metabolism of americium-241 and absorbed doses in organs

DOE Office of Scientific and Technical Information (OSTI.GOV)

Buldakov, L.A.; Kalmykova, Z.I.

1979-12-01

The metabolism of soluble americium-241 compounds administered to dogs by inhalation was studied over a period of 6.5 years. The rate of excretion of americium-241 in feces and urine, organ uptake, and survival were monitored.

Effects of low doses of americium 241 on animals

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rudnitskaya, E.I.; Moskalev, Yu.I.

1979-10-01

The long term effects of low doses of americium 241 on dogs and rats were investigated. Americium chloride was administered intravenously to dogs and intraperitoneally to rats in varying doses. The biological radiation effects were determined at autopsy. Survival times were reported.

PROCESS FOR SEPARATING AMERICIUM AND CURIUM FROM RARE EARTH ELEMENTS

DOEpatents

Baybarz, R.D.; Lloyd, M.H.

1963-02-26

This invention relates to methods of separating americium and curium values from rare earth values. In accordance with the invention americium, curium, and rare earth values are sorbed on an anion exchange resin. A major portion of the rare earth values are selectively stripped from the resin with a concentrated aqueous solution of lithium chloride, and americium, curium, and a minor portion of rare earth values are then stripped from the resin with a dilute aqueous solution of lithium chloride. The americium and curium values are further purified by increasing the concentration of lithium chloride in the solution to at least 8 molar and selectively extracting rare earth values from the resulting solution with a monoalkylphosphoric acid. (AEC)

Americium-241 uptake by Bahiagrass as influenced by soil type, lime, and organic matter

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hoyt, G.D.; Adriano, D.C.

1979-07-01

Availability of /sup 241/Am to bahiagrass (Paspalum notatum), a major forage crop in the southeastern US, was studied under greenhouse conditions using two soil types, two rates of lime, and four rates of organic matter. The plants were grown in pots until three clippings were obtained. Americium-241 concentrations in plant tissues from the unlimed Dothan (24% clay) soil were, on the average, approximately twice as high as those from unlimed Troup (10% clay) soil. Lime significantly reduced /sup 241/Am uptake from both soils. The americium concentration ratios (americium concentration in dry plant tissue/average americium concentration in dry soil) for limedmore » treatments were, in general, one order of magnitude lower than those for unlimed treatments. Organic matter, added to the soils as bermuda grass hay, somewhat reduced /sup 241/Am uptake, especially when added at high rates in unlimed soils. The effect of lime on uptake could be attributed to immobilization of americium ions external to the roots as a result of decreased solubility of this radionuclide and/or antagonistic effect of increased calcium ion concentration in the soil solution on americium ions. The effect of organic matter on uptake could be attributed to its fixing capacity for metals.« less

10 CFR 32.59 - Same: Leak testing of each source.

Code of Federal Regulations, 2013 CFR

2013-01-01

... kilobecquerels (0.1 microcurie) of americium-241 or radium-226 before transferring the source to a general... capable of detecting 0.185 kilobecquerel (0.005 microcurie) of americium-241 or radium-226. If a source has been shown to be leaking or losing more than 0.185 kilobecquerel (0.005 microcurie) of americium...

10 CFR 32.59 - Same: Leak testing of each source.

Code of Federal Regulations, 2012 CFR

2012-01-01

... kilobecquerels (0.1 microcurie) of americium-241 or radium-226 before transferring the source to a general....185 kilobecquerel (0.005 microcurie) of americium-241 or radium-226. If this test discloses more than... leaking or losing americium-241 or radium-226 and shall not be transferred to a general licensee under...

10 CFR 32.59 - Same: Leak testing of each source.

Code of Federal Regulations, 2014 CFR

2014-01-01

... kilobecquerels (0.1 microcurie) of americium-241 or radium-226 before transferring the source to a general... capable of detecting 0.185 kilobecquerel (0.005 microcurie) of americium-241 or radium-226. If a source has been shown to be leaking or losing more than 0.185 kilobecquerel (0.005 microcurie) of americium...

Removal of plutonium and americium from alkaline waste solutions

DOEpatents

Schulz, Wallace W.

1979-01-01

High salt content, alkaline waste solutions containing plutonium and americium are contacted with a sodium titanate compound to effect removal of the plutonium and americium from the alkaline waste solution onto the sodium titanate and provide an effluent having a radiation level of less than 10 nCi per gram alpha emitters.

Optimization of Uranium-Doped Americium Oxide Synthesis for Space Application.

PubMed

Vigier, Jean-François; Freis, Daniel; Pöml, Philipp; Prieur, Damien; Lajarge, Patrick; Gardeur, Sébastien; Guiot, Antony; Bouëxière, Daniel; Konings, Rudy J M

2018-04-16

Americium 241 is a potential alternative to plutonium 238 as an energy source for missions into deep space or to the dark side of planetary bodies. In order to use the 241 Am isotope for radioisotope thermoelectric generator or radioisotope heating unit (RHU) production, americium materials need to be developed. This study focuses on the stabilization of a cubic americium oxide phase using uranium as the dopant. After optimization of the material preparation, (Am 0.80 U 0.12 Np 0.06 Pu 0.02 )O 1.8 has been successfully synthesized to prepare a 2.96 g pellet containing 2.13 g of 241 Am for fabrication of a small scale RHU prototype. Compared to the use of pure americium oxide, the use of uranium-doped americium oxide leads to a number of improvements from a material properties and safety point of view, such as good behavior under sintering conditions or under alpha self-irradiation. The mixed oxide is a good host for neptunium (i.e., the 241 Am daughter element), and it has improved safety against radioactive material dispersion in the case of accidental conditions.

Actinide-contaminated Skin: Comparing Decontamination Efficacy of Water, Cleansing Gels, and DTPA Gels.

PubMed

Tazrart, A; Bolzinger, M A; Lamart, S; Coudert, S; Angulo, J F; Jandard, V; Briançon, S; Griffiths, N M

2018-07-01

Skin contamination by alpha-emitting actinides is a risk to workers during nuclear fuel production and reactor decommissioning. Also, the list of items for potential use in radiological dispersal devices includes plutonium and americium. The actinide chemical form is important and solvents such as tributyl phosphate, used to extract plutonium, can influence plutonium behavior. This study investigated skin fixation and efficacy of decontamination products for these actinide forms using viable pig skin in the Franz cell diffusion system. Commonly used or recommended decontamination products such as water, cleansing gel, diethylenetriamine pentaacetic acid, or octadentate hydroxypyridinone compound 3,4,3-LI(1,2-HOPO), as well as diethylenetriamine pentaacetic acid hydrogel formulations, were tested after a 2-h contact time with the contaminant. Analysis of skin samples demonstrated that more plutonium nitrate is bound to skin as compared to plutonium-tributyl phosphate, and fixation of americium to skin was also significant. The data show that for plutonium-tributyl phosphate all the products are effective ranging from 80 to 90% removal of this contaminant. This may be associated with damage to the skin by this complex and suggests a mechanical/wash-out action rather than chelation. For removal of americium and plutonium, both Trait Rouge cleansing gel and diethylenetriamine pentaacetic acid are better than water, and diethylenetriamine pentaacetic acid hydrogel is better than Osmogel. The different treatments, however, did not significantly affect the activity in deeper skin layers, which suggests a need for further improvement of decontamination procedures. The new diethylenetriamine pentaacetic acid hydrogel preparation was effective in removing americium, plutonium, and plutonium-tributyl phosphate from skin; such a formulation offers advantages and thus merits further assessment.

Reports of the second All-Union conference on the chemistry of transplutonium elements (Dmitrovgrad, June 21-23, 1963)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Not Available

1987-05-01

The nine papers presented at this conference cover the following topics: the systematization, condensed description, and prediction of sets of anion exchange extraction constants on the basis of their statistical computer treatment; characteristics and uses of solid extractants containing D2EHPA and TBP for separating the transplutonium elements; enrichment of americium 242m and americium 242 by the Szilard-Chalmers method; an x-ray diffraction pattern analysis for transplutonium compounds; the radiation chemistry of americium; and the effects of alpha irradiation on the behavior of americium in perchlorate solutions.

Investigation of factors affecting the quality of americium electroplating.

PubMed

Trdin, M; Benedik, L; Samardžija, Z; Pihlar, B

2012-09-01

Four different electrolyte solutions were used in the electrodeposition of americium and their influences on the quality of the thin layer of deposited americium isotopes in combination with three different cathode disc materials were investigated. The relations between alpha spectral resolution and disc surface properties were established. Copyright © 2012 Elsevier Ltd. All rights reserved.

Rapid Radiochemical Method for Americium-241 in Building ...

EPA Pesticide Factsheets

Technical Fact Sheet Analysis Purpose: Qualitative analysis Technique: Alpha spectrometry Method Developed for: Americium-241 in building materials Method Selected for: SAM lists this method for qualitative analysis of americium-241 in concrete or brick building materials. Summary of subject analytical method which will be posted to the SAM website to allow access to the method.

Airborne plutonium-239 and americium-241 concentrations measured from the 125-meter Hanford Meteorological Tower

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sehmel, G.A.

1978-01-01

Airborne plutonium-239 and americium-241 concentrations and fluxes were measured at six heights from 1.9 to 122 m on the Hanford meteorological tower. The data show that plutonium-239 was transported on nonrespirable and small particles at all heights. Airborne americium-241 concentrations on small particles were maximum at the 91 m height.

Process chemistry of americium-241

DOE Office of Scientific and Technical Information (OSTI.GOV)

Navratil, J.D.

1983-01-01

Americium-241, one of the most useful actinide isotopes, is produced as a by-product of plutonium scrap recovery operations. Rocky Flats has supplied high purity americium oxide to the US Department of Energy's Isotope Pool since 1962. Over the years, the evolving separation and purification processes have included such diverse operations as ion exchange, aqueous precipitation, and both molten-salt and organic-solvent extraction.

[Assessment of the distribution in the body and the dose on the respiratory tract and organs after single, short-term and long-term inhalation of americium-241].

PubMed

Malykhin, V M

1991-04-01

On the basis of comparison of publications on accidental human intake of americium-241 and animal experimental studies dosimetric characteristics were obtained reflecting the dynamics of accumulation, formation of the dose on the organs and parts of the respiratory tract, as well as of the 24-hour elimination from the organism of the mentioned radionuclide following single, short- and long-term administration of americium-241 from the air. Results were obtained with the use of computers for quantitative modelling of the most complete metabolic transport scheme of americium.

SEPARATION OF AMERICIUM FROM PROMETHIUM

DOEpatents

Pressly, R.E.

1959-07-01

Promethium-147 is separated from americium in acidic aqueous solution by adding fluosilicic acid to the solution, heating the solution to form a promethium precipitate and separating the precipitate from solution. The precipitate is then re-dissolved by ihe addition of boric acid and nitric acid, and re-precipitated by the addition of fluosilicic acid. This procedure is repeated six or more times to obtain a relatively americium-free promeihium precipitate. Americium may be separately recovered from the supernatant liquids. This process is applicable to the recovery of promethium from fission-product solutions which have been allowed to decay for a period of two to four years.

Environmental impact of a teratogenic actinide: a case study of americium-241

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wang, J.; Yang, J.Y.

1985-10-16

Americium-241 is widely used as a radiation source, but it also has some potential risk if taken into the body. Although the radiotoxicity of americium-241 is small compared to other transuranic actinides, its effects on the reproductive system and on development of the placenta are more damaging than the effects of plutonium-239. A previous report based on a worst-case scenario involving a hypothetical fire accident in a contaminated facility indicated that there could have been a significant impact on nearby residents from a unit release of americium-241 via atmospheric dispersion. However, because the facility is located in a rural regionmore » where most drinking water supplies are drawn from private wells, it is believed that deposition of americium-241 from the atmosphere might also have impacts via the groundwater pathway by infiltration of rainwater. In this analysis, a three-dimensional analytical mathematical model is used to assess several aspects of americium-241 contamination of groundwater, including radioactive transformation, advection, dispersion, and soil sorption. Simulation results indicate that no significant radiological impacts would occur to the nearby residents via the groundwater pathway. 15 refs., 2 figs., 2 tabs.« less

Behavior of Americium in Simulated Wounds in Nonhuman Primates

DOE PAGES

Poudel, Deepesh; Guilmette, Raymond A.; Bertelli, Luiz; ...

2017-06-01

An americium solution injected intramuscularly into several nonhuman primates (NHPs) was found to behave differently than predicted by the wound models described in the NCRP Report 156. This was because the injection was made along with a citrate solution, which is known to be more soluble than chlorides, oxides, or nitrates on which the NCRP Report was based. We developed a multi-exponential wound model specific to the injected americium solution based on the retention in the intramuscular sites. The model was coupled with the americium systemic model to interpret the urinary excretion data and assess the intake, and it wasmore » determined that the models were adequate to predict early urinary excretion in most cases but unable to predict late urinary excretion. This was attributed to the differences in the systemic handling of americium between humans and nonhuman primates. Furthermore, information on the type of wounds, solubility, particle size, mass, chemical form, etc., should always be considered when performing wound dosimetry.« less

Aqueous Chloride Operations Overview: Plutonium and Americium Purification/Recovery

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gardner, Kyle Shelton; Kimball, David Bryan; Skidmore, Bradley Evan

These are a set of slides intended for an information session as part of recruiting activities at Brigham Young University. It gives an overview of aqueous chloride operations, specifically on plutonium and americium purification/recovery. This presentation details the steps taken perform these processes, from plutonium size reduction, dissolution, solvent extraction, oxalate precipitation, to calcination. For americium recovery, it details the CLEAR (chloride extraction and actinide recovery) Line, oxalate precipitation and calcination.

Metabolism of americium-241 in man: an unusual case of internal contamination of a child and his father

DOE Office of Scientific and Technical Information (OSTI.GOV)

Cohen, N.; Lo Sasso, T.; Wrenn, M.E.

1979-10-05

The metabolism of americium-241 has been studied during an 8-year period in an adult male and his son who, at the ages of 50 and 4 years, respectively, were accidentally and unknowingly contaminated within their home by means of inhalation. Chelation therapy with calcium trisodium pentetate was more effective in enhancing the removal of americium-241 from the child than from the father.

Metabolism of americium-241 in man: an unusual case of internal contamination of a child and his father.

PubMed

Cohen, N; Sasso, T L; Wrenn, M E

1979-10-05

The metabolism of americium-241 has been studied during an 8-year period in an adult male and his son who, at the ages of 50 and 4 years, respectively, were accidentally and unknowingly contaminated within their home by means of inhalation. Chelation therapy with calcium trisodium pentetate was more effective in enhancing the removal of americium-241 from the child than from the father.

Environmental impacts of the release of a transuranic actinide, americium-241, from a contaminated facility

DOE Office of Scientific and Technical Information (OSTI.GOV)

Want, J.; Merry-Libby, P.

1985-10-29

Americium-241 is widely used as a radiation source, but it also has some potential risk if taken into the body because of its high dose conversion factor. Although the radiotoxicity of americium-241 is small compared to other transuranic actinides, its effects on the reproductive system and on development of the placenta are more damaging than the effects of plutonium-239. In Ohio, a gemologist's laboratory was contaminated with americium-241. Prior to decontamination of the laboratory, potential radiological impacts to the surrounding environment were assessed. A hypothetical fire accident resulting in a unit release (1 curie) was assumed. Potential radiological impacts weremore » simulated using an atmospheric dispersion and dosimetry model with local meteorological data, population census data, and detailed information regarding the neighborhood. The results indicate that there could have been a significant impact on nearby residents from americium-241 via atmospheric dispersion if a major catastrophic release had occurred prior to contamination and decommissioning of the laboratory. 14 refs., 3 figs., 2 tabs.« less

Apoptosis of rat kidney cells after 241-americium administration.

PubMed

Labéjof, L; Berry, J P; Duchambon, P; Poncy, J L; Galle, P

1998-01-01

Tumors induction by americium is well known but there are no data on the biological effects of this radionucleide at subcellular level. In order to study the possible ultrastructural lesions induced by this element, a group of rats were injected with 241-Americium-citrate (9 kBq), once a week for five weeks and sacrificed 7 days after the last injection. We describe the alterations observed in the cortex kidney using cytochemical (TUNEL reaction) and histochemical (PAS staining) methods for light microscopy as well as electron microscopy techniques. Various types of lesions were detected: condensation of nuclear chromatine, fragmentation of the nuclei, swollen mitochondria, disappearance of mitochondrial crests and skrinking of the cytoplasm. This study clearly demonstrated the induction of apoptosis by americium in rat cortex kidney cells.

The Most Useful Actinide Isotope: Americium-241.

ERIC Educational Resources Information Center

Navratil, James D.; And Others

1990-01-01

Reviewed is the discovery, nuclear and chemical properties, and uses of an isotope of Americium (Am-241). Production and separation techniques used in industry are emphasized. Processes are illustrated in flow sheets. (CW)

SEPARATION OF CURIUM AND AMERICIUM

DOEpatents

Fields, P.R.; Isaac, N.M.

1962-02-20

Curium and americium are contained in an anhydrous molten salt medium having a low melting point. Curium is preferentially extracted from the molten salt by a hot organic solvent containing preferably less than 10% alkyl phosphate. (AEC)

Synthesis of actinide nitrides, phosphides, sulfides and oxides

DOEpatents

Van Der Sluys, William G.; Burns, Carol J.; Smith, David C.

1992-01-01

A process of preparing an actinide compound of the formula An.sub.x Z.sub.y wherein An is an actinide metal atom selected from the group consisting of thorium, uranium, plutonium, neptunium, and americium, x is selected from the group consisting of one, two or three, Z is a main group element atom selected from the group consisting of nitrogen, phosphorus, oxygen and sulfur and y is selected from the group consisting of one, two, three or four, by admixing an actinide organometallic precursor wherein said actinide is selected from the group consisting of thorium, uranium, plutonium, neptunium, and americium, a suitable solvent and a protic Lewis base selected from the group consisting of ammonia, phosphine, hydrogen sulfide and water, at temperatures and for time sufficient to form an intermediate actinide complex, heating said intermediate actinide complex at temperatures and for time sufficient to form the actinide compound, and a process of depositing a thin film of such an actinide compound, e.g., uranium mononitride, by subliming an actinide organometallic precursor, e.g., a uranium amide precursor, in the presence of an effectgive amount of a protic Lewis base, e.g., ammonia, within a reactor at temperatures and for time sufficient to form a thin film of the actinide compound, are disclosed.

Radionuclide Basics: Americium-241

EPA Pesticide Factsheets

Americium (chemical symbol Am) is a man-made radioactive metal that is solid under normal conditions. Exposure to a significant amount of Am-241 is generally unlikely. Small amounts are found in the soil, plants and water from nuclear weapons testing.

Chemistry of americium

DOE Office of Scientific and Technical Information (OSTI.GOV)

Schulz, W.W.

1976-01-01

Essential features of the descriptive chemistry of americium are reviewed. Chapter titles are: discovery, atomic and nuclear properties, collateral reading, production and uses, chemistry in aqueous solution, metal, alloys, and compounds, and, recovery, separation, purification. Author and subject indexes are included. (JCB)

THE PREPARATION, PROPERTIES, AND USES OF AMERICIUM-241, ALPHA-, GAMMA-, AND NEUTRON SOURCES

DOE Office of Scientific and Technical Information (OSTI.GOV)

Strain, J.E.; Leddicotte, G.W.

1962-09-01

A study was made of the preparation of alpha, gamma, and neutron sources using the long-lived radioisotope of americium, Am/sup 241/. Americium-241 is an artificiallyproduced radioelement which has a half-life of 462 plus or minus 10 years and decays to Np/sup 237/ by alpha emission followed by low-energy gamma emission. The high specific activity of americium-241 (7.0 x 10/sup 9/ d/m/mg) combined with its reasonably long half-life makes it ideally sulted for the preparation of radioactive sources. The chemical and physical properties of Am/ sup 241/ and the physical manipulations involved in fabricating alpha, gamma, and neutron sources are generallymore » described in this report. Uses for each type of source are discussed and data are presented to indicate the respective properties and usefulness of each source type. (auth)« less

A Hybrid Density Functional Study of Atomic Hydrogen and Oxygen Adsorptions on the (0001) Surface of Non-Magnetic DHCP Americium

NASA Astrophysics Data System (ADS)

Amdani-Moten, Shafaq; Atta-Fynn, Raymond; Ray, Asok

2010-03-01

As our group have recently shown^+, hybrid density functional theory (HDFT) which replaces a fraction (40%) of approximate DFT exchange with exact Hartree-Fock exchange yield structural, magnetic, and electronic properties for Americium-I that are in excellent agreement with experimental data. As a natural progression, ab initio calculations for atomic adsorptions on the (0001) surface of non-magnetic americium have been performed using HDFT. The americium surface is modeled by a seven-layer slab using inversion symmetry consisting of one atom per layer and non-magnetic ABAC stacking arrangement of these layers. Top, bridge, hcp and fcc chemisorption sites have been investigated with energies optimized with respect to the adatom distance from the surface. Details of the chemisorptions processes as well as comparisons of different sites will be presented. ^+ R. Atta-Fynn and A. K. Ray, Chemical Physics Letters, 482, 223-227 (2009).

The TRUSPEAK Concept: Combining CMPO and HDEHP for Separating Trivalent Lanthanides from the Transuranic Elements

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lumetta, Gregg J.; Gelis, Artem V.; Braley, Jenifer C.

2013-04-08

Combining octyl(phenyl)-N,N-diisobutyl-carbamoylmethyl-phosphine oxide (CMPO) and bis-(2-ethylhexyl) phosphoric acid (HDEHP) into a single process solvent for separating transuranic elements from liquid high-level waste is explored. Co-extraction of americium and the lanthanide elements from nitric acid solution is possible with a solvent mixture consisting of 0.1-M CMPO plus 1-M HDEHP in n-dodecane. Switching the aqueous-phase chemistry to a citrate-buffered solution of diethylene triamine pentaacetic acid (DTPA) allows for selective stripping of americium, separating it from the lanthanide elements. Potential strategies for managing molybdenum and zirconium (both of which co-extract with americium and the lanthanides) have been developed. The work presented here demonstratesmore » the feasibility of combining CMPO and HDEHP into a single extraction solvent for recovering americium from high-level waste and its separation from the lanthanides.« less

TRANSURANIC STUDIES STATUS AND PROBLEM STATEMENT

DOE Office of Scientific and Technical Information (OSTI.GOV)

Leuze, R E

1959-04-29

The purpose of the Transuranics Program is to develop separation processes for the transuranic elements, primarily those produced by long-term neutron irradiation of Pu/sup 239/. The program includes laboratory process development, pilot-plant process testing, processing of 10 kg of Pu/sup 239/ irradiated to greater than 99% burn-up for plutonium and americium-curium recovery, and processing the reirradiated plutonium and americium-curium fractions. The proposed method for processing highly irradiated plutonium is: (1) plutonium-aluminum alloy dissolution in HNO/sub 3/; (2) plutonium recovery by TBP extraction; (3) americium, curium, and rare-earth extraction by TBP from neutral nitrate solution; (4) partial rare-earth removal (primarily lanthanum)more » by americium-curium extraction into 100% TBP from 15M HNO/sub 3/; (5) additional rare-earth removal by extraction in 0.48M mono-2-ethylhexylphosphoric acid from 12M HCl; and (6) americium-curium purification by chloride anion exchange. Processing through the 100% TBP, 15M HNO/sub 3/ cycle can be carried out in the Power Reactor Fuel Reprocessing Pilot Plant. New facilities are proposed 15M HNO/ sub 3/ cycle can be carried out in the Power Reactor Fuel Reprocessing Pilot Plant. New facilities are proposed for laboratory process development studies and the final processing of the transplutonic elements. (auth)« less

Porous metal oxide microspheres from ion exchange resin

NASA Astrophysics Data System (ADS)

Picart, S.; Parant, P.; Caisso, M.; Remy, E.; Mokhtari, H.; Jobelin, I.; Bayle, J. P.; Martin, C. L.; Blanchart, P.; Ayral, A.; Delahaye, T.

2015-07-01

This study is devoted to the synthesis and the characterization of porous metal oxide microsphere from metal loaded ion exchange resin. Their application concerns the fabrication of uranium-americium oxide pellets using the powder-free process called Calcined Resin Microsphere Pelletization (CRMP). Those mixed oxide ceramics are one of the materials envisaged for americium transmutation in sodium fast neutron reactors. The advantage of such microsphere precursor compared to classical oxide powder is the diminution of the risk of fine dissemination which can be critical for the handling of highly radioactive powders such as americium based oxides and the improvement of flowability for the filling of compaction chamber. Those millimetric oxide microspheres incorporating uranium and americium were synthesized and characterizations showed a very porous microstructure very brittle in nature which occurred to be adapted to shaping by compaction. Studies allowed to determine an optimal heat treatment with calcination temperature comprised between 700-800 °C and temperature rate lower than 2 °C/min. Oxide Precursors were die-pressed into pellets and then sintered under air to form regular ceramic pellets of 95% of theoretical density (TD) and of homogeneous microstructure. This study validated thus the scientific feasibility of the CRMP process to prepare bearing americium target in a powder free manner.

Comparing the 2,2'-Biphenylenedithiophosphinate Binding of Americium with Neodymium and Europium

DOE PAGES

Cross, Justin N.; Macor, Joseph A.; Bertke, Jeffery A.; ...

2016-09-15

Advancing our understanding of the minor actinides (Am, Cm) versus lanthanides is key for developing advanced nuclear-fuel cycles. Here in this paper, we describe the preparation of (NBu 4)Am[S 2P( tBu 2C 12H 6)] 4 and two isomorphous lanthanide complexes, namely one with a similar ionic radius (i.e., Nd III) and an isoelectronic one (Eu III). The results include the first measurement of an Am-S bond length, with a mean value of 2.921(9) Å, by single-crystal X-ray diffraction. Comparison with the Eu III and Nd III complexes revealed subtle electronic differences between the complexes of Am III and the lanthanides.

Thromboelastograms of dogs with acute and subacute lesions due to inhalation of americium 241 and plutonium 239 nitrates

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kalmykova, Z.I.

1978-01-01

The effects of inhalation of americium 241 and plutonium 231 on the clotting mechanism of dogs were investigated. Thromboelastograms of whole venous blood were used as the method for studying coagulation properties.

Accumulation, organ distribution, and excretion kinetics of ²⁴¹Am in Mayak Production Association workers.

PubMed

Suslova, Klara G; Sokolova, Alexandra B; Efimov, Alexander V; Miller, Scott C

2013-03-01

Americium-241 (²⁴¹Am) is the second most significant radiation hazard after ²³⁹Pu at some of the Mayak Production Association facilities. This study summarizes current data on the accumulation, distribution, and excretion of americium compared with plutonium in different organs from former Mayak PA workers. Americium and plutonium were measured in autopsy and bioassay samples and correlated with the presence or absence of chronic disease and with biological transportability of the aerosols encountered at different workplaces. The relative accumulation of ²⁴¹Am was found to be increasing in the workers over time. This is likely from ²⁴¹Pu that increases with time in reprocessed fuel and from the increased concentrations of ²⁴¹Am and ²⁴¹Pu in inhaled alpha-active aerosols. While differences were observed in lung retention with exposures to different industrial compounds with different transportabilities (i.e., dioxide and nitrates), there were no significant differences in lung retention between americium and plutonium within each transportability group. In the non-pulmonary organs, the highest ratios of ²⁴¹Am/²⁴¹Am + SPu were observed in the skeleton. The relative ratios of americium in the skeleton versus liver were significantly greater than for plutonium. The relative amounts of americium and plutonium found in the skeleton compared with the liver were even greater in workers with documented chronic liver diseases. Excretion rates of ²⁴¹Am in ‘‘healthy’’ workers were estimated using bioassay and autopsy data. The data suggest that impaired liver function leads to reduced hepatic ²⁴¹Am retention, leading to increased ²⁴¹Am excretion.

Electronic Structure of Actinides under Pressure

NASA Astrophysics Data System (ADS)

Johansson, Borje

2006-03-01

The series of heavy radioactive elements known as the actinides all have similar elemental properties. However, when the volume per atom in the condensed phase is illustrated as a function of atomic number, perhaps the most dramatic anomaly in the periodic table becomes apparent. The atomic volume of americium is almost 50% larger than it is for the preceding element plutonium. For the element after americium, curium, the atomic volume is very close to that of americium. The same holds also for the next elements berkelium and californium. Accordingly from americium and onwards the actinides behave very similar to the corresponding rare-earth elements - a second lanthanide series of metallic elements can be identified. This view is strongly supported by the fact that all these elements adopt the dhcp structure, a structure typical for the lanthanides. The reason for this behavior is found in the behavior of the 5f electrons. For the earlier actinides, up to and including plutonium, the 5f electrons form metallic states and contribute most significantly to the bonding. In Np and Pu they even dominate the bonding, while all of a sudden they become localized in Am, very much like the 4f electrons in the lanthanide series, and contribute no longer to the cohesion. This withdrawal of 5f bonding gives rise to the large volume expansion between plutonium and americium. This difference between the light and heavy actinide suggests that it would be most worthwhile to strongly compress the transplutonium elements, thereby forcing the individual 5f electron wave functions into strong contact with each other (overlap). Recently high pressure experiments have been performed for americium and curium and dramatic crystal structure changes have been observed. These results and other high pressure data will be discussed in relation to the basic electronic structure of these elements.

Total and Compound Formation Cross Sections for Americium Nuclei: Recommendations for Coupled-Channels Calculations

DOE Office of Scientific and Technical Information (OSTI.GOV)

Escher, J. E.

Calculations for total cross sections and compound-nucleus (CN) formation cross sections for americium isotopes are described, for use in the 2017 NA-22 evaluation effort. The code ECIS 2006 was used in conjunction with Frank Dietrich's wrapper `runtemplate'.

[Rapid analysis of the radionuclides plutonium and americium-241 in soils].

PubMed

Egorov, A V; Klochkova, N V

2009-01-01

The paper shows it possible to perform a rapid analysis of the isotopes of plutomium and americium-241. The basis of the developed rapid analysis is X-spectrometric determination of the amount of plutonium isotopes and gamma-spectrometric determination of the radionuclide 241AM.

In situ characterization of uranium and americium oxide solid solution formation for CRMP process: first combination of in situ XRD and XANES measurements.

PubMed

Caisso, Marie; Picart, Sébastien; Belin, Renaud C; Lebreton, Florent; Martin, Philippe M; Dardenne, Kathy; Rothe, Jörg; Neuville, Daniel R; Delahaye, Thibaud; Ayral, André

2015-04-14

Transmutation of americium in heterogeneous mode through the use of U1-xAmxO2±δ ceramic pellets, also known as Americium Bearing Blankets (AmBB), has become a major research axis. Nevertheless, in order to consider future large-scale deployment, the processes involved in AmBB fabrication have to minimize fine particle dissemination, due to the presence of americium, which considerably increases the risk of contamination. New synthesis routes avoiding the use of pulverulent precursors are thus currently under development, such as the Calcined Resin Microsphere Pelletization (CRMP) process. It is based on the use of weak-acid resin (WAR) microspheres as precursors, loaded with actinide cations. After two specific calcinations under controlled atmospheres, resin microspheres are converted into oxide microspheres composed of a monophasic U1-xAmxO2±δ phase. Understanding the different mechanisms during thermal conversion, that lead to the release of organic matter and the formation of a solid solution, appear essential. By combining in situ techniques such as XRD and XAS, it has become possible to identify the key temperatures for oxide formation, and the corresponding oxidation states taken by uranium and americium during mineralization. This paper thus presents the first results on the mineralization of (U,Am) loaded resin microspheres into a solid solution, through in situ XAS analysis correlated with HT-XRD.

Plutonium-239 and americium-241 uptake by plants from soil. Final report

DOE Office of Scientific and Technical Information (OSTI.GOV)

Brown, K.W.

1979-03-01

Alfalfa was grown in soil contaminated with plutonium-239 dioxide (239PuO2) at a concentration of 29.7 nanocuries per gram (nCi/g). In addition to alfalfa, radishes, wheat, rye, and tomatoes were grown in soils contaminated with americium-241 nitrate (241Am(NO3)3) at a concentration of 189 nCi/g. The length of exposure varied from 52 days for the radishes to 237 days for the alfalfa. The magnitude of plutonium incorporation by the alfalfa as indicated by the concentration ratio, 0.0000025, was similar to previously reported data using other chemical forms of plutonium. The results did indicate, however, that differences in the biological availability of plutoniummore » isotopes do exist. All of the species exposed to americium-241 assimilated and translocated this radioisotope to the stem, leaf, and fruiting structures. The magnitude of incorporation as signified by the concentration ratios varied from 0.00001 for the wheat grass to 0.0152 for the radishes. An increase in the uptake of americium also occurred as a function of time for four of the five plant species. Evidence indicates that the predominant factor in plutonium and americium uptake by plants may involve the chelation of these elements in soils by the action of compounds such as citric acid and/or other similar chelating agents released from plant roots.« less

Solubility of Plutonium (IV) Oxalate During Americium/Curium Pretreatment

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rudisill, T.S.

1999-08-11

Approximately 15,000 L of solution containing isotopes of americium and curium (Am/Cm) will undergo stabilization by vitrification at the Savannah River Site (SRS). Prior to vitrification, an in-tank pretreatment will be used to remove metal impurities from the solution using an oxalate precipitation process. Material balance calculations for this process, based on solubility data in pure nitric acid, predict approximately 80 percent of the plutonium in the solution will be lost to waste. Due to the uncertainty associated with the plutonium losses during processing, solubility experiments were performed to measure the recovery of plutonium during pretreatment and a subsequent precipitationmore » process to prepare a slurry feed for a batch melter. A good estimate of the plutonium content of the glass is required for planning the shipment of the vitrified Am/Cm product to Oak Ridge National Laboratory (ORNL).The plutonium solubility in the oxalate precipitation supernate during pretreatment was 10 mg/mL at 35 degrees C. In two subsequent washes with a 0.25M oxalic acid/0.5M nitric acid solution, the solubility dropped to less than 5 mg/mL. During the precipitation and washing steps, lanthanide fission products in the solution were mostly insoluble. Uranium, and alkali, alkaline earth, and transition metal impurities were soluble as expected. An elemental material balance for plutonium showed that greater than 94 percent of the plutonium was recovered in the dissolved precipitate. The recovery of the lanthanide elements was generally 94 percent or higher except for the more soluble lanthanum. The recovery of soluble metal impurities from the precipitate slurry ranged from 15 to 22 percent. Theoretically, 16 percent of the soluble oxalates should have been present in the dissolved slurry based on the dilution effects and volumes of supernate and wash solutions removed. A trace level material balance showed greater than 97 percent recovery of americium-241 (from the beta dec ay of plutonium-241) in the dissolved precipitate, a value consistent with the recovery of europium, the americium surrogate.In a subsequent experiment, the plutonium solubility following an oxalate precipitation to simulate the preparation of a slurry feed for a batch melter was 21 mg/mL at 35 degrees C. The increase in solubility compared to the value measured during the pretreatment experiment was attributed to the increased nitrate concentration and ensuing increase in plutonium complexation. The solubility of the plutonium following a precipitant wash with 0.1M oxalic acid was unchanged. The recovery of plutonium from the precipitate slurry was greater than 97 percent allowing an estimation that approximately 92 percent of the plutonium in Tank 17.1 will report to the glass. The behavior of the lanthanides and soluble metal impurities was consistent with the behavior seen during the pretreatment experiment. A trace level material balance showed that 99.9 percent of the americium w as recovered from the precipitate slurry. The overall recovery of americium from the pretreatment and feed preparation processes was greater than 97 percent, which was consistent with the measured recovery of the europium surrogate.« less

EPA Method: Rapid Radiochemical Method for Americium-241, Radium-226, Plutonium-238/-239, Radiostronium, and Isotopic Uranium in Water for Environmental Restoration Following Homeland Security Events

EPA Pesticide Factsheets

SAM lists this method for the qualitative determination of Americium-241, Radium-226, Plutonium-238, Plutonium-239 and isotopic uranium in drinking water samples using alpha spectrometry and radiostrontium using beta counting.

Glenn T. Seaborg - Contributions to Advancing Science

Science.gov Websites

. Documents: The First Weighing of Plutonium (Atomic Number 94); DOE Technical Report; September 1967 The New Element Americium (Atomic Number 95); DOE Technical Report; January 1948 The New Element Curium (Atomic Number 96); DOE Technical Report; January 1948 Frontiers of Chemistry for Americium and Curium; DOE

10 CFR 32.59 - Same: Leak testing of each source.

Code of Federal Regulations, 2011 CFR

2011-01-01

... Energy NUCLEAR REGULATORY COMMISSION SPECIFIC DOMESTIC LICENSES TO MANUFACTURE OR TRANSFER CERTAIN ITEMS... kilobecquerels (0.1 microcurie) of americium-241 or radium-226 before transferring the source to a general... leaking or losing americium-241 or radium-226 and shall not be transferred to a general licensee under...

10 CFR 32.59 - Same: Leak testing of each source.

Code of Federal Regulations, 2010 CFR

2010-01-01

... Energy NUCLEAR REGULATORY COMMISSION SPECIFIC DOMESTIC LICENSES TO MANUFACTURE OR TRANSFER CERTAIN ITEMS... kilobecquerels (0.1 microcurie) of americium-241 or radium-226 before transferring the source to a general... leaking or losing americium-241 or radium-226 and shall not be transferred to a general licensee under...

Auger electron and characteristic energy loss spectra for electro-deposited americium-241

NASA Astrophysics Data System (ADS)

Varma, Matesh N.; Baum, John W.

1983-07-01

Auger electron energy spectra for electro-deposited americium-241 on platinum substrate were obtained using a cylindrical mirror analyzer. Characteristic energy loss spectra for this sample were also obtained at primary electron beam energies of 990 and 390 eV. From these measurements PI, PII, and PIII energy levels for americium-241 are determined. Auger electron energies are compared with theoretically calculated values. Minimum detectability under the present condition of sample preparation and equipment was estimated at approximately 1.2×10-8 g/cm2 or 3.9×10-8 Ci/cm2. Minimum detectability for plutonium-239 under similar conditions was estimated at about 7.2×10-10 Ci/cm2.

Combined radiochemical procedure for determination of plutonium, americium and strontium-90 in the soil samples from SNTS

NASA Astrophysics Data System (ADS)

Kazachevskii, I. V.; Lukashenko, S. N.; Chumikov, G. N.; Chakrova, E. T.; Smirin, L. N.; Solodukhin, V. P.; Khayekber, S.; Berdinova, N. M.; Ryazanova, L. A.; Bannyh, V. I.; Muratova, V. M.

1999-01-01

The results of combined radiochemical procedure for the determination of plutonium, americium and90Sr (via measurement of90Y) in the soil samples from SNTS are presented. The processes of co-precipitation of these nuclides with calcium fluoride in the strong acid solutions have been investigated. The conditions for simultaneous separation of americium and yttrium using extraction chromatography have been studied. It follows from analyses of real soil samples that the procedure developed provides the chemical recovery of plutonium and yttrium in the range of 50-95% and 60-95%, respectively. The execution of the procedure requires 3.5 working days including a sample decomposition study.

Cleaning up the Legacy of the Cold War: Plutonium Oxides and the Role of Synchrotron Radiation Research

DOE Office of Scientific and Technical Information (OSTI.GOV)

Clark, David Lewis

2015-01-21

The deceptively simple binary formula of AnO 2 belies an incredibly complex structural nature, and propensity to form mixed-valent, nonstoichiometric phases of composition AnO 2±x. For plutonium, the very formation of PuO 2+x has challenged a long-established dogma, and raised fundamental questions for long-term storage and environmental migration. This presentation covers two aspects of Los Alamos synchrotron radiation studies of plutonium oxides: (1) the structural chemistry of laboratory-prepared AnO 2+x systems (An = U, Pu; 0 ≤ x ≤ 0.25) determined through a combination of x-ray absorption fine structure spectroscopy (XAFS) and x-ray scattering of laboratory prepared samples; and (2)more » the application of synchrotron radiation towards the decontamination and decommissioning of the Rocky Flats Environmental Technology Site. Making the case for particle transport mechanisms as the basis of plutonium and americium mobility, rather than aqueous sorption-desorption processes, established a successful scientific basis for the dominance of physical transport processes by wind and water. The scientific basis was successful because it was in agreement with general theory on insolubility of PuO 2 in oxidation state IV, results of ultrafiltration analyses of field water/sediment samples, XAFS analyses of soil, sediment, and concrete samples, and was also in general agreement with on-site monitoring data. This understanding allowed Site contractors to rapidly move to application of soil erosion and sediment transport models as the means of predicting plutonium and americium transport, which led to design and application of site-wide soil erosion control technology to help control downstream concentrations of plutonium and americium in streamflow.« less

Enhanced ionization efficiency in TIMS analyses of plutonium and americium using porous ion emitters

DOE PAGES

Baruzzini, Matthew L.; Hall, Howard L.; Watrous, Matthew G.; ...

2016-12-05

Investigations of enhanced sample utilization in thermal ionization mass spectrometry (TIMS) using porous ion emitter (PIE) techniques for the analyses of trace quantities of americium and plutonium were performed. Repeat ionization efficiency (i.e., the ratio of ions detected to atoms loaded on the filament) measurements were conducted on sample sizes ranging from 10–100 pg for americium and 1–100 pg for plutonium using PIE and traditional (i.e., a single, zone-refined rhenium, flat filament ribbon with a carbon ionization enhancer) TIMS filament sources. When compared to traditional filaments, PIEs exhibited an average boost in ionization efficiency of ~550% for plutonium and ~1100%more » for americium. A maximum average efficiency of 1.09% was observed at a 1 pg plutonium sample loading using PIEs. Supplementary trials were conducted using newly developed platinum PIEs to analyze 10 pg mass loadings of plutonium. As a result, platinum PIEs exhibited an additional ~134% boost in ion yield over standard PIEs and ~736% over traditional filaments at the same sample loading level.« less

Uptake and effects of americium-241 on a brackishwater amphipod

NASA Astrophysics Data System (ADS)

Hoppenheit, M.; Murray, C. N.; Woodhead, D. S.

1980-03-01

The present paper reports the results of experimental work undertaken using the brackish-water amphipod Gammarus duebeni duebeni and the transuranium nuclide americium-241. Data on the accumulation of this actinide showed that the larger fraction of the total body burden is associated with the exoskeleton. It was found that the body burden remained constant in the range pH 8.0 6.5 even though the water concentrations changed markedly. It would thus appear that the concept of a concentration factor should be re-examined and it is proposed that a factor should be defined in terms of environmental and chemical parameters which represent the bioavailable fraction of the actinide. The effect of americium on survival and moulting was studied at two activity concentrations; the dose rates and absorbed doses under the experimental conditions employed have been estimated. The differences in survival rates between the control and irradiated groups were statistically analyzed and the significant difference at the higher concentration is believed to be due to a synergism between physiological stress and radiotoxicity of americium rather than the chemical toxicity of the element.

Experimental findings on actinide recovery utilizing oxidation by peroxydisulfate followed by ion exchange: Fuel cycle research & development

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hobbs, D. T.; Shehee, T. C.

2015-08-31

Our research seeks to determine if inorganic ion-exchange materials can be exploited to provide effective minor actinide (Am, Cm) separation from lanthanides. Previous work has established that a number of inorganic and UMOF ion-exchange materials exhibit varying affinities for actinides and lanthanides, which may be exploited for effective separations. During FY15, experimental work focused on investigating methods to oxidize americium in dilute nitric and perchloric acid with subsequent ion-exchange performance measurements of ion exchangers with the oxidized americium in dilute nitric acid. Ion-exchange materials tested included a variety of alkali titanates. Americium oxidation testing sought to determine the influence thatmore » other redox active components may have on the oxidation of Am III. Experimental findings indicated that Ce III, Np V, and Ru II are oxidized by peroxydisulfate, but there are no indications that the presence of Ce III, Np V, and Ru II affected the rate or extent of americium oxidation at the concentrations of peroxydisulfate being used.« less

On the influence of the americium isotopic vector on the cooling time of minor actinides bearing blankets in fast reactors

NASA Astrophysics Data System (ADS)

Kooyman, Timothée; Buiron, Laurent; Rimpault, Gerald

2018-05-01

In the heterogeneous minor actinides transmutation approach, the nuclei to be transmuted are loaded in dedicated targets often located at the core periphery, so that long-lived heavy nuclides are turned into shorter-lived fission products by fission. To compensate for low flux level at the core periphery, the minor actinides content in the targets is set relatively high (around 20 at.%), which has a negative impact on the reprocessing of the targets due to their important decay heat level. After a complete analysis of the main contributors to the heat load of the irradiated targets, it is shown here that the choice of the reprocessing order of the various feeds of americium from the fuel cycle depends on the actual limit for fuel reprocessing. If reprocessing of hot targets is possible, it is more interesting to reprocess first the americium feed with a high 243Am content in order to limit the total cooling time of the targets, while if reprocessing of targets is limited by their decay heat, it is more interesting to wait for an increase in the 241Am content before loading the americium in the core. An optimization of the reprocessing order appears to lead to a decrease of the total cooling time by 15 years compared to a situation where all the americium feeds are mixed together when two feeds from SFR are considered with a high reprocessing limit.

10 CFR 32.57 - Calibration or reference sources containing americium-241 or radium-226: Requirements for license...

Code of Federal Regulations, 2013 CFR

2013-01-01

... design; (3) Details of the method of incorporation and binding of the americium-241 or radium-226 in the source; (4) Procedures for and results of prototype testing of sources, which are designed to contain... additional information, including experimental studies and tests, required by the Commission to facilitate a...

10 CFR 32.57 - Calibration or reference sources containing americium-241 or radium-226: Requirements for license...

Code of Federal Regulations, 2012 CFR

2012-01-01

... design; (3) Details of the method of incorporation and binding of the americium-241 or radium-226 in the source; (4) Procedures for and results of prototype testing of sources, which are designed to contain... additional information, including experimental studies and tests, required by the Commission to facilitate a...

10 CFR 32.57 - Calibration or reference sources containing americium-241 or radium-226: Requirements for license...

Code of Federal Regulations, 2010 CFR

2010-01-01

... design; (3) Details of the method of incorporation and binding of the americium-241 or radium-226 in the source; (4) Procedures for and results of prototype testing of sources, which are designed to contain... additional information, including experimental studies and tests, required by the Commission to facilitate a...

10 CFR 32.57 - Calibration or reference sources containing americium-241 or radium-226: Requirements for license...

Code of Federal Regulations, 2014 CFR

2014-01-01

... design; (3) Details of the method of incorporation and binding of the americium-241 or radium-226 in the source; (4) Procedures for and results of prototype testing of sources, which are designed to contain... additional information, including experimental studies and tests, required by the Commission to facilitate a...

10 CFR 32.57 - Calibration or reference sources containing americium-241 or radium-226: Requirements for license...

Code of Federal Regulations, 2011 CFR

2011-01-01

... design; (3) Details of the method of incorporation and binding of the americium-241 or radium-226 in the source; (4) Procedures for and results of prototype testing of sources, which are designed to contain... additional information, including experimental studies and tests, required by the Commission to facilitate a...

10 CFR 32.102 - Schedule C-prototype tests for calibration or reference sources containing americium-241 or...

Code of Federal Regulations, 2011 CFR

2011-01-01

... 10 Energy 1 2011-01-01 2011-01-01 false Schedule C-prototype tests for calibration or reference sources containing americium-241 or radium-226. 32.102 Section 32.102 Energy NUCLEAR REGULATORY COMMISSION SPECIFIC DOMESTIC LICENSES TO MANUFACTURE OR TRANSFER CERTAIN ITEMS CONTAINING BYPRODUCT MATERIAL Generally...

Final Radiological Assessment of External Exposure for CLEAR-Line Americium Recovery Operations

DOE Office of Scientific and Technical Information (OSTI.GOV)

Davis, Adam C.; Belooussova, Olga N.; Hetrick, Lucas Duane

2014-11-12

Los Alamos National Laboratory is currently planning to implement an americium recovery program. The americium, ordinarily isotopically pure 241Am, would be extracted from existing Pu materials, converted to an oxide and shipped to support fabrication of americium oxide-beryllium neutron sources. These operations would occur in the currently proposed Chloride Extraction and Actinide Recovery (CLEAR) line of glove boxes. This glove box line would be collocated with the currently-operational Experimental Chloride Extraction Line (EXCEL). The focus of this document is to provide an in-depth assessment of the currently planned radiation protection measures and to determine whether or not further design workmore » is required to satisfy design-goal and ALARA requirements. Further, this document presents a history of americium recovery operations in the Department of Energy and high-level descriptions of the CLEAR line operations to provide a basis of comparison. Under the working assumptions adopted by this study, it was found that the evaluated design appears to mitigate doses to a level that satisfies the ALARA-in-design requirements of 10 CFR 835 as implemented by the Los Alamos National Laboratory procedure P121. The analyses indicate that extremity doses would also meet design requirements. Dose-rate calculations were performed using the radiation transport code MCNP5 and doses were estimated using a time-motion study developed in consort with the subject matter expert. A copy of this report and all supporting documentation are located on the Radiological Engineering server at Y:\\Rad Engineering\\2013 PROJECTS\\TA-55 Clear Line.« less

National low-level waste management program radionuclide report series, Volume 14: Americium-241

DOE Office of Scientific and Technical Information (OSTI.GOV)

Winberg, M.R.; Garcia, R.S.

1995-09-01

This report, Volume 14 of the National Low-Level Waste Management Program Radionuclide Report Series, discusses the radiological and chemical characteristics of americium-241 ({sup 241}Am). This report also includes discussions about waste types and forms in which {sup 241}Am can be found and {sup 241}Am behavior in the environment and in the human body.

Effect of Americium-241 Content on Plutonium Radiation Source Terms

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rainisch, R.

1998-12-28

The management of excess plutonium by the US Department of Energy includes a number of storage and disposition alternatives. Savannah River Site (SRS) is supporting DOE with plutonium disposition efforts, including the immobilization of certain plutonium materials in a borosilicate glass matrix. Surplus plutonium inventories slated for vitrification include materials with elevated levels of Americium-241. The Am-241 content of plutonium materials generally reflects in-growth of the isotope due to decay of plutonium and is age-dependent. However, select plutonium inventories have Am-241 levels considerably above the age-based levels. Elevated levels of americium significantly impact radiation source terms of plutonium materials andmore » will make handling of the materials more difficult. Plutonium materials are normally handled in shielded glove boxes, and the work entails both extremity and whole body exposures. This paper reports results of an SRS analysis of plutonium materials source terms vs. the Americium-241 content of the materials. Data with respect to dependence and magnitude of source terms on/vs. Am-241 levels are presented and discussed. The investigation encompasses both vitrified and un-vitrified plutonium oxide (PuO2) batches.« less

Americium alloys with gold and copper

NASA Astrophysics Data System (ADS)

Radchenko, V. M.; Ryabinin, M. A.; Chernakova, T. A.; Tomilin, S. V.

2010-03-01

Presented are results of the production and X-ray examination of micro-samples of americium-241 compounds with gold and copper produced by high-temperature condensation of metal americium vapor onto corresponding substrates. No mutual solubility of the investigated system components was revealed at room temperature. The following three intermetallic compounds were revealed in the Am-Au system: Au6Am with tetragonal lattice of the Au6Sm structural type, AuAm with orthorhombic lattice of the CuCe structural type and AuAm with cubic lattice. The Am-Cu system showed the intermetallic compound Cu5Am (Cu7Am) with a hexagonal lattice of the Cu5Ca(Cu7Tb) structure type. An effect of the 241Am nuclide alpha-activity on the crystal structure of the produced intermetallide was studied.

Effect of americium-241 alpha-particles on the dose-response of chromosome aberrations in human lymphocytes analysed by fluorescence in situ hybridization.

PubMed

Barquinero, J F; Stephan, G; Schmid, E

2004-02-01

To evaluate by the fluorescent in-situ hybridization (FISH) technique the dose-response and intercellular distribution of alpha-particle-induced chromosome aberrations. In particular, the validity of using the yield of characteristic types of chromosome abnormalities in stable cells as quantitative indicators for retrospective dose reconstruction has been evaluated. Monolayers of human peripheral lymphocytes were exposed at doses from 0.02 to 1 Gy to alpha-particles emitted from a source of americium-241. The most probable energy of the alpha-particles entering the cells was 2.7 MeV. FISH painting was performed using DNA probes for chromosomes 2, 4 and 8 in combination with a pan-centromeric probe. In complete first-division cells, identified by harlequin staining, aberrations involving painted target chromosomal material were recorded as well as aberrations involving only unpainted chromosomal material. In total, the percentage of complex aberrations was about 35% and no dose dependence was observed. When complex-type exchanges were reduced to simple base types, the different cell distributions were clearly over-dispersed, and the linear coefficients of the dose-effect curves for translocations were significantly higher than for dicentrics. For past dose reconstruction, only a few complex aberrations were in stable cells. The linear coefficient obtained for transmissible aberrations in stable cells was more than seven times lower than that obtained in all analysed cells, i.e. including unstable cells. FISH-based analysis of complex rearrangements allows discrimination between partial-body exposures to low-linear energy transfer radiation and high-linear energy transfer exposures. In assessing past or chronic exposure to alpha-particles, the use of a dose-effect curve obtained by FISH-based translocation data, which had not excluded data determined in unstable cells, would underestimate the dose. Insertions are ineffective biomarkers because their frequency is too low.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Syarifah, Ratna Dewi, E-mail: syarifah.physics@gmail.com; Suud, Zaki, E-mail: szaki@fi.itb.ac.id

Design study of small Pressurized Water Reactors (PWRs) core loaded with uranium nitride fuel (UN) and mixed nitride fuel (UN-PuN), Pa-231 as burnable poison, and Americium has been performed. Pa-231 known as actinide material, have large capture cross section and can be converted into fissile material that can be utilized to reduce excess reactivity. Americium is one of minor actinides with long half life. The objective of adding americium is to decrease nuclear spent fuel in the world. The neutronic analysis results show that mixed nitride fuel have k-inf greater than uranium nitride fuel. It is caused by the additionmore » of Pu-239 in mixed nitride fuel. In fuel fraction analysis, for uranium nitride fuel, the optimum volume fractions are 45% fuel fraction, 10% cladding and 45% moderator. In case of UN-PuN fuel, the optimum volume fractions are 30% fuel fraction, 10% cladding and 60% coolant/ moderator. The addition of Pa-231 as burnable poison for UN fuel, enrichment U-235 5%, with Pa-231 1.6% has k-inf more than one and excess reactivity of 14.45%. And for mixed nitride fuel, the lowest value of reactivity swing is when enrichment (U-235+Pu) 8% with Pa-231 0.4%, the excess reactivity value 13,76%. The fuel pin analyze for the addition of Americium, the excess reactivity value is lower than before, because Americium absorb the neutron. For UN fuel, enrichment U-235 8%, Pa-231 1.6% and Am 0.5%, the excess reactivity is 4.86%. And for mixed nitride fuel, when enrichment (U-235+Pu) 13%, Pa-231 0.4% and Am 0.1%, the excess reactivity is 11.94%. For core configuration, it is better to use heterogeneous than homogeneous core configuration, because the radial power distribution is better.« less

Selective separation of americium from europium using 2,9-bis(triazine)-1,10-phenanthrolines in ionic liquids: a new twist on an old story

DOE Office of Scientific and Technical Information (OSTI.GOV)

Williams, Neil J.; Dehaudt, Jeremy; Bryantsev, Vyacheslav S.

Bis-triazine phenanthrolines have shown great promise for f-block metal separations, attributable to their highly preorganized structure, nitrogen donors, and more enhanced covalent bonding with actinides over lanthanides. However, their limited solubility in traditional solvents remains a technological bottleneck. Here in this paper we report our recent work using a simple 2,9-bis(triazine)-1,10-phenanthroline (Me-BTPhen) dissolved in an ionic liquid (IL), demonstrating the efficacy of IL extraction systems for the selective separation of americium from europium, achieving separation factors in excess of 7500 and selectively removing up to 99% of the americium. Characterization of the coordination environment was performed using a combination ofmore » X-ray absorption fine structure spectroscopy (XAFS) and density functional theory (DFT) calculations.« less

Selective separation of americium from europium using 2,9-bis(triazine)-1,10-phenanthrolines in ionic liquids: a new twist on an old story

DOE PAGES

Williams, Neil J.; Dehaudt, Jeremy; Bryantsev, Vyacheslav S.; ...

2017-02-10

Bis-triazine phenanthrolines have shown great promise for f-block metal separations, attributable to their highly preorganized structure, nitrogen donors, and more enhanced covalent bonding with actinides over lanthanides. However, their limited solubility in traditional solvents remains a technological bottleneck. Here in this paper we report our recent work using a simple 2,9-bis(triazine)-1,10-phenanthroline (Me-BTPhen) dissolved in an ionic liquid (IL), demonstrating the efficacy of IL extraction systems for the selective separation of americium from europium, achieving separation factors in excess of 7500 and selectively removing up to 99% of the americium. Characterization of the coordination environment was performed using a combination ofmore » X-ray absorption fine structure spectroscopy (XAFS) and density functional theory (DFT) calculations.« less

New Concepts for Compact Space Reactor Power Systems for Space Based Radar Applications: A Feasibility Study

DTIC Science & Technology

1989-12-01

SPENT FUEL REPROCESSING COULD ALSO BE EMPLOYED IRRADIATION EXPERIENCE - EXTREMELY LIMITED - JOINT US/UK PROGRAM (ONGOING) - TUI/KFK PROGRAM (CANCELED...only the use of off-the-shelf technologies. For example, conventional fuel technology (uranium dioxide), conventional thermionic conversion...advanced fuel (Americium oxide, A1TI2O3) and advanced thermionic conversion. Concept C involves use of an advanced fuel (Americium oxide, Arri203

Heterogeneity Effects in Plutonium Contaminated Soil

DTIC Science & Technology

2009-03-01

masses up to one kilogram once the ratio of Americium - 241 (Am- 241 ) and plutonium concentrations was established (Rademacher, 2001). Alpha...with a sample number and tared weight with a non-smearing marker. A standard control was then set using a point source of Americium - 241 on an aluminum...During the fire the weapons grade plutonium (Pu- 239, Pu-240, and Pu- 241 ) ignited and was released into the surrounding area, due to both

Rapid Testing of Fresh Concrete

DTIC Science & Technology

1975-05-01

in Figure 2. The cement content gage, on the other hand, employs a low energy source, Americium - 241 (60 Kev), for which the photoelectric absorption...holder are also shown schemati- cally in Figure 5. The probe contains a 14 millicurie Americium - 241 radioisotope source, a 1-in. diameter by 1-in...lower the sensitivity but the greater the penetration depth. A compromise is obtained using Am- 241 , a long-lived source (458 yr half-life) of 60

Brachytherapy devices and methods employing americium-241

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gray, L. A.

1985-04-16

Sources and methods for radiation therapy, particularly brachytherapy, employing americium-241 (60 keV gamma emission and 433 year half-life) provide major advantages for radiotherapy, including simplified radiation protection, dose reduction to healthy tissue, increased dose to tumor, and improved dose distributions. A number of apparent drawbacks and unfavorable considerations including low gamma factor, high self-absorption, increased activity required and alpha-particle generation leading to helium gas pressure buildup and potential neutron contamination in the generated radiation are all effectively dealt with and overcome through recognition of subtle favorable factors unique to americium-241 among brachytherapy sources and through suitable constructional techniques. Due tomore » an additional amount of radiation, in the order of 50%, provided primarily to nearby regions as a result of Compton scatter in tissue and water, higher dose rates occur than would be predicted by conventional calculations.« less

Actinide Oxidation State and O/M Ratio in Hypostoichiometric Uranium-Plutonium-Americium U0.750Pu0.246Am0.004O2-x Mixed Oxides.

PubMed

Vauchy, Romain; Belin, Renaud C; Robisson, Anne-Charlotte; Lebreton, Florent; Aufore, Laurence; Scheinost, Andreas C; Martin, Philippe M

2016-03-07

Innovative americium-bearing uranium-plutonium mixed oxides U1-yPuyO2-x are envisioned as nuclear fuel for sodium-cooled fast neutron reactors (SFRs). The oxygen-to-metal (O/M) ratio, directly related to the oxidation state of cations, affects many of the fuel properties. Thus, a thorough knowledge of its variation with the sintering conditions is essential. The aim of this work is to follow the oxidation state of uranium, plutonium, and americium, and so the O/M ratio, in U0.750Pu0.246Am0.004O2-x samples sintered for 4 h at 2023 K in various Ar + 5% H2 + z vpm H2O (z = ∼ 15, ∼ 90, and ∼ 200) gas mixtures. The O/M ratios were determined by gravimetry, XAS, and XRD and evidenced a partial oxidation of the samples at room temperature. Finally, by comparing XANES and EXAFS results to that of a previous study, we demonstrate that the presence of uranium does not influence the interactions between americium and plutonium and that the differences in the O/M ratio between the investigated conditions is controlled by the reduction of plutonium. We also discuss the role of the homogeneity of cation distribution, as determined by EPMA, on the mechanisms involved in the reduction process.

Comparative XRPD and XAS study of the impact of the synthesis process on the electronic and structural environments of uranium–americium mixed oxides

DOE Office of Scientific and Technical Information (OSTI.GOV)

Prieur, D., E-mail: dam.prieur@gmail.com; Lebreton, F.; Martin, P.M.

2015-10-15

Uranium–americium mixed oxides are potential compounds to reduce americium inventory in nuclear waste via a partitioning and transmutation strategy. A thorough assessment of the oxygen-to-metal ratio is paramount in such materials as it determines the important underlying electronic structure and phase relations, affecting both thermal conductivity of the material and its interaction with the cladding and coolant. In 2011, various XAS experiments on U{sub 1−x}Am{sub x}O{sub 2±δ} samples prepared by different synthesis methods have reported contradictory results on the charge distribution of U and Am. This work alleviates this discrepancy. The XAS results confirm that, independently of the synthesis process,more » the reductive sintering of U{sub 1−x}Am{sub x}O{sub 2±δ} leads to the formation of similar fluorite solid solution indicating the presence of Am{sup +III} and U{sup +V} in equimolar proportions. - Graphical abstract: Formation of (U{sup IV/V},Am{sup III})O{sup 2} solid solution by sol–gel and by powder metallurgy. - Highlights: • Uranium–americium mixed oxides were synthesized by sol–gel and powder metallurgy. • Fluorite solid solutions with similar local environment have been obtained. • U{sup V} and Am{sup III} are formed in equimolar proportions.« less

Vertical and horizontal fluxes of plutonium and americium in the western Mediterranean and the Strait of Gibraltar.

PubMed

León Vintró, L; Mitchell, P I; Condren, O M; Downes, A B; Papucci, C; Delfanti, R

1999-09-30

New data on the vertical distributions of plutonium and americium in the waters of the western Mediterranean and the Strait of Gibraltar are examined in terms of the processes governing their delivery to, transport in and removal from the water column within the basin. Residence times for plutonium and americium in surface waters of approximately 15 and approximately 3 years, respectively, are deduced, and it is shown that by the mid 1990s only approximately 35% of the 239,240Pu and approximately 5% of the 241Am deposited as weapons fallout still resided in the water column. Present 239,240Pu inventories in the water column and the underlying sediments are estimated to be approximately 25 TBq and approximately 40 TBq, respectively, which reconcile well with the time-integrated fallout deposition in this zone, taken to be approximately 69 TBq. The data show that there are significant net outward fluxes of plutonium and americium from the basin through the Strait of Gibraltar at the present time. These appear to be compensated by net inward fluxes of similar magnitude through the Strait of Sicily. Thus, the time-integrated fallout deposition in the western basin can be accounted for satisfactorily in terms of present water column and sediment inventories. Enhanced scavenging on the continental shelves, as evidenced by the appreciably higher transuranic concentrations in shelf sediments, supports this contention.

The prospect of uranium nitride (UN) and mixed nitride fuel (UN-PuN) for pressurized water reactor

NASA Astrophysics Data System (ADS)

Syarifah, Ratna Dewi; Suud, Zaki

2015-09-01

Design study of small Pressurized Water Reactors (PWRs) core loaded with uranium nitride fuel (UN) and mixed nitride fuel (UN-PuN), Pa-231 as burnable poison, and Americium has been performed. Pa-231 known as actinide material, have large capture cross section and can be converted into fissile material that can be utilized to reduce excess reactivity. Americium is one of minor actinides with long half life. The objective of adding americium is to decrease nuclear spent fuel in the world. The neutronic analysis results show that mixed nitride fuel have k-inf greater than uranium nitride fuel. It is caused by the addition of Pu-239 in mixed nitride fuel. In fuel fraction analysis, for uranium nitride fuel, the optimum volume fractions are 45% fuel fraction, 10% cladding and 45% moderator. In case of UN-PuN fuel, the optimum volume fractions are 30% fuel fraction, 10% cladding and 60% coolant/ moderator. The addition of Pa-231 as burnable poison for UN fuel, enrichment U-235 5%, with Pa-231 1.6% has k-inf more than one and excess reactivity of 14.45%. And for mixed nitride fuel, the lowest value of reactivity swing is when enrichment (U-235+Pu) 8% with Pa-231 0.4%, the excess reactivity value 13,76%. The fuel pin analyze for the addition of Americium, the excess reactivity value is lower than before, because Americium absorb the neutron. For UN fuel, enrichment U-235 8%, Pa-231 1.6% and Am 0.5%, the excess reactivity is 4.86%. And for mixed nitride fuel, when enrichment (U-235+Pu) 13%, Pa-231 0.4% and Am 0.1%, the excess reactivity is 11.94%. For core configuration, it is better to use heterogeneous than homogeneous core configuration, because the radial power distribution is better.

Design of Alpha Voltaic Power Source Using Americium 241 (241Am) and Diamond with a Power Density of 10 mW/cm3

DTIC Science & Technology

2017-10-19

GaN) was calculated and compared . Alpha-voltaic energy converters were designed in diamond and GaN based on the energy deposition calculations...Example Power Source Two example device designs are calculated and compared . A diamond device containing 2 charge collection regions (Schottky and p...ARL-TR-8189 ● OCT 2017 US Army Research Laboratory Design of Alpha-Voltaic Power Source Using Americium-241 (241Am) and Diamond

Colloid formation during waste form reaction: Implications for nuclear waste disposal

USGS Publications Warehouse

Bates, J. K.; Bradley, J.; Teetsov, A.; Bradley, C. R.; Buchholtz ten Brink, Marilyn R.

1992-01-01

Insoluble plutonium- and americium-bearing colloidal particles formed during simulated weathering of a high-level nuclear waste glass. Nearly 100 percent of the total plutonium and americium in test ground water was concentrated in these submicrometer particles. These results indicate that models of actinide mobility and repository integrity, which assume complete solubility of actinides in ground water, underestimate the potential for radionuclide release into the environment. A colloid-trapping mechanism may be necessary for a waste repository to meet long-term performance specifications.

Inspection report of unauthorized possession and use of unsealed americium-241 and subsequent confiscation, J. C. Haynes Company, Newark, Ohio

DOE Office of Scientific and Technical Information (OSTI.GOV)

Not Available

1985-11-01

This US Nuclear Regulatory Commission report documents the circumstances surrounding the March 26, 1985, confiscation and subsequent decontamination activities related to the use of unauthorized quantities of americium-241 at the John C. Haynes Company (licensee) of Newark, Ohio. It focuses on the period from early February to July 26, 1985. The incident started when NRC Region III recieved information that John C. Haynes possessed unauthorized quantities of americium-241 and was conducting unauthorized activities (diamond irradiation). By July 26, 1985, the decontamination activities at the licensee's laboratory were concluded. The licensee's actions with diamond irradiation resulted in contamination in restricted andmore » unrestricted areas of the facility. The confiscation and decontamination activities required the combined efforts of NRC, Federal Bureau of Investigation, US Department of Energy, Oak Ridge Associated Universities, the State of Ohio, and the US Environmental Protection Agency. The report describes the factual information and significant findings associated with the confiscation and decontamination activities.« less

An LDA+U study of the photoemission spectra of ground state phase of americium and curium

NASA Astrophysics Data System (ADS)

Islam, Md; Ray, Asok

2009-03-01

We have investigated the photoemission spectra and other ground state properties such as equilibrium volume and bulk modulus of dhcp americium and the density of states and magnetic properties of dhcp curium using LDA+U method. Our calculations show that spin polarized americium is energetically favorable but spin degenerate configuration produces experimental quantities much better than that calculated using spin polarized configuration. The DOS calculated using LDA+U with both non-magnetic and spin polarized configurations is compared and the non-magnetic DOS is shown to be in good agreement with experimental photoemission spectra when U=4.5 eV. In spin polarized case, U is observed to increase the splitting between occupied and unoccupied bands by enhancing Stoner parameter. The results are shown to be in good agreement with that calculated using dynamical mean field theory for these two heavy actinides. For curium, exchange interaction appears to play the dominant role in its magnetic stability.

The biodistribution and toxicity of plutonium, americium and neptunium.

PubMed

Taylor, D M

1989-07-15

In the nuclear fuel cycle the transuranic radionuclides plutonium-239, americium-241 and neptunium-237 would probably present the most serious hazard to human health if released into the environment. Despite differences in their solution chemistry the three elements exhibit remarkable similarity in their biochemical behaviour, apparently sharing similar transport pathways in blood and cells. After entering the blood the elements deposit predominantly in liver and skeleton, where retention appears to be prolonged, with half-times of the order of years. The principal late effects of all three radionuclides are the induction of cancers of bone, lung or liver. For the latter tumours the induction risk per unit radiation dose appears similar for the three radionuclides. But in bone there are indications that, due to microscopic differences in the distribution of the alpha-particle radiation dose, the efficiency of bone cancer induction may increase in the order americium-241 less than plutonium-239 less than neptunium-237. No case of human cancer induced by these radionuclides is known.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Marshall, R.S.

A simple in-line americium assay instrument (AAI) was installed at an americium recovery process area at LASL for use in process development and for providing process control information. The AAI counts 59.5-keV /sup 241/Am gamma rays, using a NaI(T1) detector and Eberline SAM II electronics. It has a useful range of 3 x 10/sup -5/ to 10 g Am/l and does not suffer from plutonium interference. Comparative analyses of samples assayed in the AAI and samples assayed by the LASL Analytical Laboratory show a combined relative standard deviation of 14%.

Rapid Method for Sodium Hydroxide Fusion of Concrete and ...

EPA Pesticide Factsheets

Technical Fact Sheet Analysis Purpose: Qualitative analysis Technique: Alpha spectrometry Method Developed for: Americium-241, plutonium-238, plutonium-239, radium-226, strontium-90, uranium-234, uranium-235 and uranium-238 in concrete and brick samples Method Selected for: SAM lists this method for qualitative analysis of americium-241, plutonium-238, plutonium-239, radium-226, strontium-90, uranium-234, uranium-235 and uranium-238 in concrete or brick building materials. Summary of subject analytical method which will be posted to the SAM website to allow access to the method.

Particulate, colloidal, and dissolved-phase associations of plutonium and americium in a water sample from well 1587 at the Rocky Flats Plant, Colorado

USGS Publications Warehouse

Harnish, R.A.; McKnight, Diane M.; Ranville, James F.

1994-01-01

In November 1991, the initial phase of a study to determine the dominant aqueous phases that control the transport of plutonium (Pu), americium (Am), and uranium (U) in surface and groundwater at the Rocky Flats Plant was undertaken by the U.S. Geological Survey. By use of the techniques of stirred-cell spiral-flow filtration and crossflow ultrafiltration, particles of three size fractions were collected from a 60-liter sample of water from well 1587 at the Rocky Flats Plant. These samples and corresponding filtrate samples were analyzed for Pu and Am. As calculated from the analysis of filtrates, 65 percent of Pu 239 and 240 activity in the sample was associated with particulate and largest colloidal size fractions. Particulate (22 percent) and colloidal (43 percent) fractions were determined to have significant activities in relation to whole-water Pu activity. Am and Pu 238 activities were too low to be analyzed. Examination and analyses of the particulate and colloidal phases indicated the presence of mineral species (iron oxyhydroxides and clay minerals) and natural organic matter that can facilitate the transport of actinides in ground water. High concentrations of the transition metals copper and zinc in the smallest colloid fractions strongly indicate a potential for organic complexation of metals, and potentially of actinides, in this size fraction.

Laboratory investigation of the role of desorption kinetics on americium transport associated with bentonite colloids.

PubMed

Dittrich, Timothy Mark; Boukhalfa, Hakim; Ware, Stuart Douglas; Reimus, Paul William

2015-10-01

Understanding the parameters that control colloid-mediated transport of radionuclides is important for the safe disposal of used nuclear fuel. We report an experimental and reactive transport modeling examination of americium transport in a groundwater-bentonite-fracture fill material system. A series of batch sorption and column transport experiments were conducted to determine the role of desorption kinetics from bentonite colloids in the transport of americium through fracture materials. We used fracture fill material from a shear zone in altered granodiorite collected from the Grimsel Test Site (GTS) in Switzerland and colloidal suspensions generated from FEBEX bentonite, a potential repository backfill material. The colloidal suspension (100 mg L(-1)) was prepared in synthetic groundwater that matched the natural water chemistry at GTS and was spiked with 5.5 × 10(-10) M (241)Am. Batch characterizations indicated that 97% of the americium in the stock suspension was adsorbed to the colloids. Breakthrough experiments conducted by injecting the americium colloidal suspension through three identical columns in series, each with mean residence times of 6 h, show that more than 95% of the bentonite colloids were transported through each of the columns, with modeled colloid filtration rates (k(f)) of 0.01-0.02 h(-1). Am recoveries in each column were 55-60%, and Am desorption rate constants from the colloids, determined from 1-D transport modeling, were 0.96, 0.98, and 0.91 h(-1) in the three columns, respectively. The consistency in Am recoveries and desorption rate constants in each column indicates that the Am was not associated with binding sites of widely-varying strengths on the colloids, as one binding site with fast kinetics represented the system accurately for all three sequential columns. Our data suggest that colloid-mediated transport of Am in a bentonite-fracture fill material system is unlikely to result in transport over long distance scales because of the ability of the fracture materials to rapidly strip Am from the bentonite colloids and the apparent lack of a strong binding site that would keep a fraction of the Am strongly-associated with the colloids. Published by Elsevier Ltd.

A LDA + U study of the photoemission spectra of the double hexagonal close packed phases of Am and Cm

NASA Astrophysics Data System (ADS)

Islam, M. Fhokrul; Ray, Asok K.

2010-05-01

We have investigated the photoemission spectra and other electronic structure properties such as equilibrium volume and bulk modulus of double hexagonal close packed (dhcp) americium and the density of states (DOS) and magnetic properties of dhcp curium using the LDA+U method. Our calculations show that spin polarized americium is energetically favorable but spin degenerate configuration produces experimental quantities significantly better than those calculated using the spin polarized configuration. The density of states calculated using LDA+U with both non-magnetic and spin polarized configurations is compared and the non-magnetic DOS is shown to be in good agreement with experimental photoemission spectra when U=4.5 eV. In spin polarized case, the onsite interaction parameter, U, is observed to increase the splitting between occupied and unoccupied bands by enhancing the Stoner parameter. The DOS of both non-magnetic americium and anti-ferromagnetic curium are shown to be in good agreement with that calculated using dynamical mean field theory for these two heavy actinides. For curium exchange interaction appears to play a dominant role in magnetic stability.

Extraction processes and solvents for recovery of cesium, strontium, rare earth elements, technetium and actinides from liquid radioactive waste

DOEpatents

Zaitsev, Boris N.; Esimantovskiy, Vyacheslav M.; Lazarev, Leonard N.; Dzekun, Evgeniy G.; Romanovskiy, Valeriy N.; Todd, Terry A.; Brewer, Ken N.; Herbst, Ronald S.; Law, Jack D.

2001-01-01

Cesium and strontium are extracted from aqueous acidic radioactive waste containing rare earth elements, technetium and actinides, by contacting the waste with a composition of a complex organoboron compound and polyethylene glycol in an organofluorine diluent mixture. In a preferred embodiment the complex organoboron compound is chlorinated cobalt dicarbollide, the polyethylene glycol has the formula RC.sub.6 H.sub.4 (OCH.sub.2 CH.sub.2).sub.n OH, and the organofluorine diluent is a mixture of bis-tetrafluoropropyl ether of diethylene glycol with at least one of bis-tetrafluoropropyl ether of ethylene glycol and bis-tetrafluoropropyl formal. The rare earths, technetium and the actinides (especially uranium, plutonium and americium), are extracted from the aqueous phase using a phosphine oxide in a hydrocarbon diluent, and reextracted from the resulting organic phase into an aqueous phase by using a suitable strip reagent.

Species-dependent chelation of (241)Am by DTPA Di-ethyl ester.

PubMed

Huckle, James E; Sadgrove, Matthew P; Mumper, Russell J; Jay, Michael

2015-04-01

Diethylenetriaminepentaacetic acid (DTPA) is an FDA-approved chelating agent for enhancing the elimination of transuranic elements such as americium from the body. Early access to therapy minimizes deposition of these radionuclides in tissues such as the bone. Due to its poor oral bioavailability, DTPA is administered as an IV injection, delaying access. Therefore, a diethyl-ester analog of DTPA, named C2E2, was synthesized as a means to increase oral absorption. As a hexadentate ligand, it was hypothesized that C2E2 was capable of binding americium directly. Therefore, the protonation constants and americium stability constant for C2E2 were determined by potentiometric titration and a solvent extraction method, respectively. C2E2 was shown to bind americium with a log K of 19.6. The concentrations of C2E2, its metabolite C2E1, and DTPA required to achieve effective binding in rat, beagle, and human plasma were studied in vitro. Dose response curves for each ligand were established, and the 50% maximal effective concentrations were determined for each species. As expected, higher concentrations of C2E2 were required to achieve the same degree of binding as DTPA. The results indicated that chelation in beagle plasma is more representative of the human response than rats. Finally, the pharmacokinetics of C2E2 were investigated in beagles, and the data was fit to a two-compartment model with elimination from the central compartment, along with first-order absorption. Based on the in vitro data, a 100 mg kg dose of C2E2 can be expected to have an effective duration of action of 3.8 h in beagles.

Species-Dependent Chelation of 241Am by DTPA Di-ethyl Ester

PubMed Central

Huckle, James E.; Sadgrove, Matthew P.; Mumper, Russell J.; Jay, Michael

2014-01-01

Diethylenetriaminepentaacetic acid (DTPA) is an FDA approved chelating agent for enhancing the elimination of transuranic elements such as americium from the body. Early access to therapy minimizes deposition of these radionuclides in tissues such as the bone. Due to its poor oral bioavailability, DTPA is administered as an IV injection, delaying access. Therefore a diethyl-ester analog of DTPA, named C2E2, was synthesized as a means to increase oral absorption. As a hexadentate ligand, it was hypothesized that C2E2 was capable of binding americium directly. Therefore, the protonation constants and americium stability constant for C2E2 were determined by potentiometric titration and a solvent extraction method, respectively. C2E2 was shown to bind americium with a log K of 19.6. The concentrations of C2E2, its metabolite C2E1, and DTPA required to achieve effective binding in rat, beagle, and human plasma were studied in vitro. Dose response curves for each ligand were established and the 50% maximal effective concentrations were determined for each species. As expected, higher concentrations of C2E2 were required to achieve the same degree of binding as DTPA. The results indicated that chelation in beagle plasma is more representative of the human response than rats. Finally, the pharmacokinetics of C2E2 were investigated in beagles and the data was fit to a two-compartment model with elimination from the central compartment, along with first-order absorption. Based on the in vitro data, a 100 mg kg−1 dose of C2E2 can be expected to have an effective duration of action of 3.8 hours in beagles. PMID:25706138

DOE Office of Scientific and Technical Information (OSTI.GOV)

Corbey, Jordan F.; Rapko, Brian M.; Wang, Zheming

Abstract The crystal structures of americium species containing a common multi-functional phosphine oxide ligand, reported for its ability to extract f elements from acidic solutions, namely 2,6-[Ph2P(O)CH2]2C5H3-NO, L, have finally been determined after over three decades of separations studies involving these species and their surrogates. The molecular compounds Am(L)(NO3)3, Am 1:1, and [Am(L)2(NO3)][NO3]2, Am 2:1, along with their neodymium and europium analogs were synthesized and characterized using single-crystal X-ray crystallography, attenuated total reflectance Fourier transform infrared (ATR) spectroscopy and luminescence spectroscopy to provide a comprehensive comparison with new and known analogous complexes.

CMPO purity tests in the TRUEX solvent using americium-241

DOE Office of Scientific and Technical Information (OSTI.GOV)

Brewer, K.N.; Herbst, R.S.; Tranter, T.J.

1993-12-01

The Transuranic Extraction (TRUEX) Process was developed by E.P. Horwitz and coworkers at Argonne National Laboratory (ANL) to separate the +4, +6, and +3 actinides from acidic aqueous solutions of nuclear wastes. Octyl (phenyl)-N-N-diisobutyl-carbamoylmethylphosphine oxide (CMPO) is the active actinide complexant used in the TRUEX solvent. CMPO is combined with tributyl phosphate (TBP) in an organic diluent, typically n-dodecane, to form the TRUEX solvent. Small quantities of impurities in the CMPO resulting from: (1) synthesis, (2) acid hydrolysis, or (3) radiolysis can result in actinide stripping problems from the solvent. The impurity, octylphenylphosphinic acid (POPPA), ia a powerful extractant atmore » low acid concentrations which may be formed during CMPO synthesis. Consequently, commercial CMPO may contain sufficient quantities of POPPA to significantly impact the stripping of actinides from the TRUEX solvent. The purpose of these tests was to (1) determine if commercially available CMPO is sufficiently pure to alleviate actinide stripping problems from the TRUEX process and (2) to determine if solvent cleanup methods are sufficient to purify the commercially purchased CMPO. Extraction and solvent cleanup methodologies used by Horwitz and coworkers at ANL were used to determine CMPO purity with {sup 241}Am. The improvement of the americium distribution coefficient in dilute nitric acid resulting from further purifying this CMPO is not significant enough to warrant additional CMPO purifying steps. The commercially purchased CMPO is found to be acceptable to use, as received, in a full-scale TRUEX process.« less

Use of DTPA for increasing the rate of elimination of plutonium-238 and americium-241 from rodents after their inhalation as the nitrates.

PubMed

Stather, J W; Stradling, G N; Gray, S A; Moody, J; Hodgson, A

1985-11-01

This study has shown that: both inhaled (2 mumol/kg) and injected (30 mumol/kg) diethylenetriaminepenta-acetic acid (DTPA) can reduce the lung deposit of 238 Pu and 241 Am inhaled as nitrate to about 1% of that in untreated controls; injection of DTPA is more effective than aerosolized DTPA for reducing deposits of 238Pu and 241Am in the liver and skeleton; combined treatment involving early inhalation of DTPA followed by repeated intravenous injections is likely to be the most effective treatment for workers who have accidentally inhaled plutonium and americium nitrates.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zalupski, Peter R.; Klaehn, John R.; Peterman, Dean R.

The feasibility of simultaneous separation of uranium, neptunium, plutonium, americium, and curium from a simulated dissolved used fuel simulant adjusted to 1.0 M nitric acid is investigated using a mixture of the soft donor bis(bis-3,5-trifluoromethyl)phenyl) dithiophosphinic acid (“0”) and the hard donor synergist trioctylphosphine oxide (TOPO) dissolved in toluene. The results reported in this work are compared to our recent demonstration of a complete actinide recovery from a simulated dissolved fuel solution using a synergistic combination of bis(o-trifluoromethylphenyl)dithiophosphinic acid (“1”) and TOPO dissolved in either toluene or trifluoromethylphenyl sulfone. While the extraction efficiency of americium was enhanced for the liquid-liquidmore » system containing “0”, enabling to accomplish a trivalent An/Ln separation at 1.0 M HNO3, the extraction of neptunium was drastically diminished, relative to “1”. The partitioning behavior of curium was also negatively impacted, introducing an effective opportunity for americium/curium separation. Radiometric and spectrophotometric studies demonstrate that the complete actinide recovery using the solvent based upon “0” and TOPO is not feasible. Additionally, the importance of radiolytic degradation processes is discussed through the comparisons of extraction properties of liquid-liquid systems based on both soft donor reagents.« less

Whole-body distribution of americium in rats for different pathways of intake.

PubMed

Doyle-Eisele, Melanie; Weber, Waylon; Melo, Dunstana R; Guilmette, Raymond A

2014-11-01

Abstract Purpose: To compare data on the whole-body distribution of americium-241 ((241)Am) in rats following intravenous injection (IV), inhalation, and wound (intramuscular injection, IM). Following exposure, each rat was placed in an individual metabolism cages for the duration of the study, 28 days (d). Urine and feces were collected daily. Tissues and organs were collected and measured. Liver and skeleton were the main sites of deposition for all routes of exposure but the content differed substantially. By 28 d, (241)Am content in liver was similar for IV and IM administrations (12 ± 4% and 14 ± 5%, respectively), which was 3-fold higher compared to inhalation. Americium-241 content in skeleton was 27% by the end of the IV study; which was 50% higher compared to the IM study and 6-fold higher compared to inhalation. The cumulative excretion in 28 d was 54% for IV (44% by feces and 10% by urine); 38% for IM (34% by feces and 4% by urine); and 84% for inhalation (83% by feces and 1% by urine). Unperturbed rat models for the three routes of administration are the baseline for evaluating the efficacy of chelating agents.

Impact of the cation distribution homogeneity on the americium oxidation state in the U0.54Pu0.45Am0.01O2-x mixed oxide

NASA Astrophysics Data System (ADS)

Vauchy, Romain; Robisson, Anne-Charlotte; Martin, Philippe M.; Belin, Renaud C.; Aufore, Laurence; Scheinost, Andreas C.; Hodaj, Fiqiri

2015-01-01

The impact of the cation distribution homogeneity of the U0.54Pu0.45Am0.01O2-x mixed oxide on the americium oxidation state was studied by coupling X-ray diffraction (XRD), electron probe micro analysis (EPMA) and X-ray absorption spectroscopy (XAS). Oxygen-hypostoichiometric Am-bearing uranium-plutonium mixed oxide pellets were fabricated by two different co-milling based processes in order to obtain different cation distribution homogeneities. The americium was generated from β- decay of 241Pu. The XRD analysis of the obtained compounds did not reveal any structural difference between the samples. EPMA, however, revealed a high homogeneity in the cation distribution for one sample, and substantial heterogeneity of the U-Pu (so Am) distribution for the other. The difference in cation distribution was linked to a difference in Am chemistry as investigated by XAS, with Am being present at mixed +III/+IV oxidation state in the heterogeneous compound, whereas only Am(IV) was observed in the homogeneous compound. Previously reported discrepancies on Am oxidation states can hence be explained by cation distribution homogeneity effects.

Laboratory investigation of the role of desorption kinetics on americium transport associated with bentonite colloids

DOE PAGES

Dittrich, Timothy Mark; Boukhalfa, Hakim; Ware, Stuart Douglas; ...

2015-07-13

Understanding the parameters that control colloid-mediated transport of radionuclides is important for the safe disposal of used nuclear fuel. We report an experimental and reactive transport modeling examination of americium transport in a groundwater–bentonite–fracture fill material system. A series of batch sorption and column transport experiments were conducted to determine the role of desorption kinetics from bentonite colloids in the transport of americium through fracture materials. We used fracture fill material from a shear zone in altered granodiorite collected from the Grimsel Test Site (GTS) in Switzerland and colloidal suspensions generated from FEBEX bentonite, a potential repository backfill material. Themore » colloidal suspension (100 mg L –1) was prepared in synthetic groundwater that matched the natural water chemistry at GTS and was spiked with 5.5 × 10 –10 M 241Am. Batch characterizations indicated that 97% of the americium in the stock suspension was adsorbed to the colloids. Breakthrough experiments conducted by injecting the americium colloidal suspension through three identical columns in series, each with mean residence times of 6 h, show that more than 95% of the bentonite colloids were transported through each of the columns, with modeled colloid filtration rates (k f) of 0.01–0.02 h –1. Am recoveries in each column were 55–60%, and Am desorption rate constants from the colloids, determined from 1-D transport modeling, were 0.96, 0.98, and 0.91 h –1 in the three columns, respectively. The consistency in Am recoveries and desorption rate constants in each column indicates that the Am was not associated with binding sites of widely-varying strengths on the colloids, as one binding site with fast kinetics represented the system accurately for all three sequential columns. As a result, our data suggest that colloid-mediated transport of Am in a bentonite-fracture fill material system is unlikely to result in transport over long distance scales because of the ability of the fracture materials to rapidly strip Am from the bentonite colloids and the apparent lack of a strong binding site that would keep a fraction of the Am strongly-associated with the colloids.« less

Sigma Team for Advanced Actinide Recycle FY2015 Accomplishments and Directions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Moyer, Bruce A.

The Sigma Team for Minor Actinide Recycle (STAAR) has made notable progress in FY 2015 toward the overarching goal to develop more efficient separation methods for actinides in support of the United States Department of Energy (USDOE) objective of sustainable fuel cycles. Research in STAAR has been emphasizing the separation of americium and other minor actinides (MAs) to enable closed nuclear fuel recycle options, mainly within the paradigm of aqueous reprocessing of used oxide nuclear fuel dissolved in nitric acid. Its major scientific challenge concerns achieving selectivity for trivalent actinides vs lanthanides. Not only is this challenge yielding to researchmore » advances, but technology concepts such as ALSEP (Actinide Lanthanide Separation) are maturing toward demonstration readiness. Efforts are organized in five task areas: 1) combining bifunctional neutral extractants with an acidic extractant to form a single process solvent, developing a process flowsheet, and demonstrating it at bench scale; 2) oxidation of Am(III) to Am(VI) and subsequent separation with other multivalent actinides; 3) developing an effective soft-donor solvent system for An(III) selective extraction using mixed N,O-donor or all-N donor extractants such as triazinyl pyridine compounds; 4) testing of inorganic and hybrid-type ion exchange materials for MA separations; and 5) computer-aided molecular design to identify altogether new extractants and complexants and theory-based experimental data interpretation. Within these tasks, two strategies are employed, one involving oxidation of americium to its pentavalent or hexavalent state and one that seeks to selectively complex trivalent americium either in the aqueous phase or the solvent phase. Solvent extraction represents the primary separation method employed, though ion exchange and crystallization play an important role. Highlights of accomplishments include: Confirmation of the first-ever electrolytic oxidation of Am(III) in a noncomplexing aqueous solution and submission of this scientific breakthrough as a paper in Science; The first-ever co-crystallization of Am(VI) with UO 2(NO 3) 2 ∙ 6H 2O, opening the door to a new approach for separating hexavalent actinides as a group; Results showing that three potentially problematic metals will not present risk in ALSEP; Improvement in ALSEP contactor stripping kinetics to acceptable performance; A comparison of centrifugal contactors vs mixer-settlers showing the former performs better in ALSEP stripping; Synthesis of new mixed N,O-donor extractants with enhanced solubility and strength for selective trivalent actinide extraction; Development of computational methods showing promise in prediction of the selectivity of new extractants for trivalent actinides vs lanthanides; An order-of-magnitude improvement in aqueous Am/Eu complexation selectivity of an alternative macrocyclic stripping agent for ALSEP, potentially enabling an option for an Am product stream free from both Ln and Cm. An alternative aqueous combination of dipicolinate complexant and malonate buffer that may present options for ALSEP and TALSPEAK (Trivalent Actinide-Lanthanide Separations by Phosphorus-reagent Extraction from Aqueous Komplexes) type separations. The ALSEP concept is advancing toward a benchtop flowsheet demonstration planned for FY 2016, and a bench-scale test bed at Idaho National Laboratory (INL) will be employed to demonstrate at least one tandem Am oxidation and separation concept. This report outlines the goals of the STAAR, significance of achieving these goals, STAAR organization around the above aims and questions, recent highlights, and future directions. The report also includes a listing of publications, reports, patents, and dissertations.« less

Sample preparation for the determination of 241Am in sediments utilizing gamma-spectroscopy.

PubMed

Ristic, M; Degetto, S; Ast, T; Cantallupi, C

2002-01-01

This paper describes a procedure developed to separate americium-241 from the bulk of a sample by coprecipitation followed by high sensitivity gamma-counting of the concentrate in a well-type detector. It enables the measurement of 241Am at low concentrations, e.g. fallout levels in soils and sediments, or where large sample sizes are not available. The method is much faster and more reliable than those involving separation from other alpha-emitters, electroplating and alpha-spectrometry. A number of tracer experiments was performed in order to optimize the conditions for coprecipitation of 241Am from sediment leachates. The general outline of the determination of americium is also given.

Monte Carlo simulation of thermal neutron flux of americium-beryllium source used in neutron activation analysis

NASA Astrophysics Data System (ADS)

Didi, Abdessamad; Dadouch, Ahmed; Bencheikh, Mohamed; Jai, Otman

2017-09-01

The neutron activation analysis is a method of exclusively elemental analysis. Its implementation of irradiates the sample which can be analyzed by a high neutron flux, this method is widely used in developed countries with nuclear reactors or accelerators of particle. The purpose of this study is to develop a prototype to increase the neutron flux such as americium-beryllium and have the opportunity to produce radioisotopes. Americium-beryllium is a mobile source of neutron activity of 20 curie, and gives a thermal neutron flux of (1.8 ± 0.0007) × 106 n/cm2 s when using water as moderator, when using the paraffin, the thermal neutron flux increases to (2.2 ± 0.0008) × 106 n/cm2 s, in the case of adding two solid beryllium barriers, the distance between them is 24 cm, parallel and symmetrical about the source, the thermal flux is increased to (2.5 ± 0.0008) × 106 n/cm2 s and in the case of multi-source (6 sources), with-out barriers, increases to (1.17 ± 0.0008) × 107 n/cm2 s with a rate of increase equal to 4.3 and with the both barriers flux increased to (1.37 ± 0.0008) × 107 n/cm2 s.

Radionuclides in ground water at the Idaho National Engineering Laboratory, Idaho

USGS Publications Warehouse

Knobel, LeRoy L.; Mann, Larry J.

1988-01-01

Sampling for radionuclides in groundwater was conducted at the Idaho National Engineering Laboratory during September to November 5 1987. Water samples from 80 wells that obtain water from the Snake River Plain aquifer and 1 well that obtains water from a shallow, discontinuous perched-water body at the Radioactive Waste Management Complex were collected and analyzed for tritium, strontium-90, plutonium-238, plutonium-239, -240 (undivided), americium-241, cesium-137, cobalt-60, and potassium-40--a naturally occurring radionuclide. The groundwater samples were analyzed at the Idaho National Engineering Laboratory in Idaho. Tritium and strontium-90 concentrations ranged from below the reporting level to 80.6 +/-0.000005 and 193 +/-5x10 to the minus eight micrograms Ci/ml, respectively. Water from a disposal well at Test Area North--which has not been used to dispose of waste water since September 1972--contained 122 +/-9x10 to the minus eleven micrograms Ci/ml of plutonium-238, 500 +/-20x10 to the minus eleven of plutonium-239, -240 (undivided), 21 +/-4x10 to the minus eleven micrograms Ci/ml of americium-241, and 750 +/-20x10 to the minus eight micrograms Ci/ml cesium-137; the presence of these radionuclides was verified by resampling and reanalysis. The disposal well had 8.9 +/-0.0000009 micrograms Ci/ml of cobalt-60 on October 28, 1987, but cobalt-60 was not detected when the well was resampled on January 11, 1988. Potassium-40 concentrations were less than the reporting level in all wells. (USGS)

Radiochemical sampling and analysis of shallow ground water and sediment at the BOMARC Missile Facility, east-central New Jersey, 1999-2000

USGS Publications Warehouse

Szabo, Zoltan; Zapecza, Otto S.; Oden, Jeannette H.; Rice, Donald E.

2005-01-01

A field sampling experiment was designed using low-flow purging with a portable pump and sample-collection equipment for the collection of water and sediment samples from observation wells screened in the Kirkwood-Cohansey aquifer system to determine radionuclide or trace-element concentrations for various size fractions. Selected chemical and physical characteristics were determined for water samples from observation wells that had not been purged for years. The sampling was designed to define any particulate, colloidal, and solution-phase associations of radionuclides or trace elements in ground water by means of filtration and ultrafiltration techniques. Turbidity was monitored and allowed to stabilize before samples were collected by means of the low-flow purging technique rather than by the traditional method of purging a fixed volume of water at high-flow rates from the observation well. A minimum of four water samples was collected from each observation well. The samples of water from each well were collected in the following sequence. (1) A raw unfiltered sample was collected within the first minutes of pumping. (2) A raw unfiltered sample was collected after at least three casing volumes of water were removed and turbidity stabilized. (3) A sample was collected after the water was filtered with a 0.45-micron filter. (4) A sample was collected after the water passed through a 0.45-micron filter and a 0.003-micron tangential-flow ultrafilter in sequence. In some cases, a fifth sample was collected after the water passed through a 0.45-micron filter and a 0.05-micron filter in sequence to test for colloids of 0.003 microns to 0.05 microns in size. The samples were analyzed for the concentration of manmade radionuclides plutonium-238 and -239 plus -240, and americium-241. The samples also were analyzed for concentrations of uranium-234, -235, and -238 to determine whether uranium-234 isotope enrichment (resulting from industrial processing) is present. A subset of samples was analyzed for concentrations of thorium-232, -230, and -228 to determine if thorium-228 isotope enrichment, also likely to result from industrial processing, is present. Concentrations of plutonium isotopes and americium-241 in the water samples were less than 0.1 picocurie per liter, the laboratory reporting level for these manmade radionuclides, with the exception of one americium-241 concentration from a filtered sample. A sequential split sample from the same well did not contain a detectable concentration of americium-241, however. Other filtered and unfiltered samples of water from the same well did not contain quantities of americium-241 nearly as high as 0.1 pCi/L. Therefore, the presence of americium-241 in a quantifiable concentration in water samples from this well could not be confirmed. Neither plutonium nor americium was detected in samples of settled sediment collected from the bottom of the wells. Concentrations of uranium isotopes (maximum of 0.05 and 0.08 picocuries per liter of uranium-238 and uranium-234, respectively) were measurable in unfiltered samples of turbid water from one well and in the settled bottom sediment from 6 wells (maximum concentrations of 0.25 and 0.20 picocuries per gram of uranium-238 and uranium-234, respectively). The uranium-234/uranium-238 isotopic ratio was near 1:1, which indicates natural uranium. The analytical results, therefore, indicate that no manmade radionuclide contamination is present in any of the well-bottom sediments, or unfiltered or filtered water samples from any of the sampled wells. No evidence of manmade radionuclide contamination was observed in the aquifer as settled or suspended particulates, colloids, or in the dissolved phase.

The uptake of plutonium-238, 239, 240, americium-241, strontium-90 and caesium-137 into potatoes.

PubMed

Popplewell, D S; Ham, G J; Johnson, T E; Stather, J W; Sumner, S A

1984-09-01

Transfer factors have been measured for 239 Pu + 240 Pu, 241 Am, 90 Sr and 137 Cs into potatoes grown in a blend of soil which included silt polluted with radioactive waste discharged into the Irish Sea. The experiment has been carried out over four seasons and attempts to assess the radiological consequences to the consumer which would arise if potatoes were to be grown in land heavily contaminated with the silt. During the course of the experiment plutonium and americium became less available for uptake, 90 Sr became slightly more available and 137 Cs remained nearly constant in its availability. The values of the transfer factors are among the lowest reported for these radionuclides into potatoes.

Synthesis and characterization of a novel aminopolycarboxylate complexant for efficient trivalent f-element differentiation: N-butyl-2-acetamide-diethylenetriamine- N, N', N", N"-tetraacetic acid

DOE Office of Scientific and Technical Information (OSTI.GOV)

Heathman, Colt R.; Grimes, Travis S.; Jansone-Popova, Santa

The novel metal ion complexant N-butyl-2-acetamide-diethylenetriamine-N,N',N",N"-tetraacetic acid (DTTA-BuA) uses an amide functionalization to increase the total ligand acidity and attain efficient 4f/5f differentiation in low pH conditions. The amide, when located on the diethylenetriamine platform containing four acetate pendant arms maintains the octadentate coordination sphere for all investigated trivalent f-elements. This compact coordination environment inhibits the protonation of LnL- complexes, as indicated by lower K 111 constants relative to the corresponding protonation site of the free ligand. For actinide ions, the enhanced stability of AnL- lowers the K 111 for americium and curium beyond the aptitude of potentiometric detection. Densitymore » functional theory computations indicate the difference in the back-donation ability of Am 3+ and Eu 3+ f-orbitals is mainly responsible for stronger proton affinity of EuL- compared to AmL-. The measured stability constants for the formation of AmL- and CmL- complexes are consistently higher, relative to ML- complexes with lanthanides of similar charge density. When compared with the conventional aminopolycarboxylate diethylenetriamine pentaacetic acid (DTPA), the modified DTTA-BuA complexant features higher ligand acidity and the important An 3+/Ln 3+ differentiation when deployed on a liquid–liquid distribution platform.« less

Complexation studies with lanthanides and humic acid analyzed by ultrafiltration and capillary electrophoresis-inductively coupled plasma mass spectrometry.

PubMed

Kautenburger, Ralf; Beck, Horst Philipp

2007-08-03

For the long-term storage of radioactive waste, detailed information about geo-chemical behavior of radioactive and toxic metal ions under environmental conditions is necessary. Humic acid (HA) can play an important role in the immobilisation or mobilisation of metal ions due to complexation and colloid formation. Therefore, we investigate the complexation behavior of HA and its influence on the migration or retardation of selected lanthanides (europium and gadolinium as homologues of the actinides americium and curium). Two independent speciation techniques, ultrafiltration and capillary electrophoresis coupled with inductively coupled plasma mass spectrometry (CE-ICP-MS) have been compared for the study of Eu and Gd interaction with (purified Aldrich) HA. The degree of complexation of Eu and Gd in 25 mg l(-1) Aldrich HA solutions was determined with a broad range of metal loading (Eu and Gd total concentration between 10(-6) and 10(-4) mol l(-1)), ionic strength of 10 mM (NaClO4) and different pH-values. From the CE-ICP-MS electropherograms, additional information on the charge of the Eu species was obtained by the use of 1-bromopropane as neutral marker. To detect HA in the ICP-MS and separate between HA complexed and non complexed metal ions in the CE-ICP-MS, we have halogenated the HA with iodine as ICP-MS marker.

Plutonium and americium in the foodchain lichen-reindeer-man

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jaakkola, T.; Hakanen, M.; Keinonen, M.

1977-01-01

The atmospheric nuclear tests have produced a worldwide fallout of transuranium elements. In addition to plutonium measurable concentrations of americium are to be found in terrestrial and aquatic environments. The metabolism of plutonium in reindeer was investigated by analyzing plutonium in liver, bone, and lung collected during 1963-1976. To determine the distribution of plutonium in reindeer all tissues of four animals of different ages were analyzed. To estimate the uptake of plutonium from the gastrointestinal tract in reindeer, the tissue samples of elk were also analyzed. Elk which is of the same genus as reindeer does not feed on lichenmore » but mainly on deciduous plants, buds, young twigs, and leaves of trees and bushes. The composition of its feed corresponds fairly well to that of reindeer during the summer. Studies on behaviour of americium along the foodchain lichen-reindeer-man were started by determining the Am-241 concentrations in lichen and reindeer liver. The Am-241 results were compared with those of Pu-239,240. The plutonium contents of the southern Finns, whose diet does not contain reindeer tissues, were determined by analyzing autopsy tissue samples (liver, lung, and bone). The southern Finns form a control group to the Lapps consuming reindeer tissues. Plutonium analyses of the placenta, blood, and tooth samples of the Lapps were performed.« less

Actinides in deer tissues at the rocky flats environmental technology site.

PubMed

Todd, Andrew S; Sattelberg, R Mark

2005-11-01

Limited hunting of deer at the future Rocky Flats National Wildlife Refuge has been proposed in U.S. Fish and Wildlife planning documents as a compatible wildlife-dependent public use. Historically, Rocky Flats site activities resulted in the contamination of surface environmental media with actinides, including isotopes of americium, plutonium, and uranium. In this study, measurements of actinides [Americium-241 (241Am); Plutonium-238 (238Pu); Plutonium-239,240 (239,240Pu); uranium-233,244 (233,234U); uranium-235,236 (235,236U); and uranium-238 (238U)] were completed on select liver, muscle, lung, bone, and kidney tissue samples harvested from resident Rocky Flats deer (N = 26) and control deer (N = 1). In total, only 17 of the more than 450 individual isotopic analyses conducted on Rocky Flats deer tissue samples measured actinide concentrations above method detection limits. Of these 17 detects, only 2 analyses, with analytical uncertainty values added, exceeded threshold values calculated around a 1 x 10(-6) risk level (isotopic americium, 0.01 pCi/g; isotopic plutonium, 0.02 pCi/g; isotopic uranium, 0.2 pCi/g). Subsequent, conservative risk calculations suggest minimal human risk associated with ingestion of these edible deer tissues. The maximum calculated risk level in this study (4.73 x 10(-6)) is at the low end of the U.S. Environmental Protection Agency's acceptable risk range.

Penetration and decontamination of americium-241 ex vivo using fresh and frozen pig skin.

PubMed

Tazrart, A; Bolzinger, M A; Moureau, A; Molina, T; Coudert, S; Angulo, J F; Briancon, S; Griffiths, N M

2017-04-01

Skin contamination is one of the most probable risks following major nuclear or radiological incidents. However, accidents involving skin contamination with radionuclides may occur in the nuclear industry, in research laboratories and in nuclear medicine departments. This work aims to measure the penetration of the radiological contaminant Americium ( 241 Am) in fresh and frozen skin and to evaluate the distribution of the contamination in the skin. Decontamination tests were performed using water, Fuller's earth and diethylene triamine pentaacetic acid (DTPA), which is the recommended treatment in case of skin contamination with actinides such as plutonium or americium. To assess these parameters, we used the Franz cell diffusion system with full-thickness skin obtained from pigs' ears, representative of human skin. Solutions of 241 Am were deposited on the skin samples. The radioactivity content in each compartment and skin layers was measured after 24 h by liquid scintillation counting and alpha spectrophotometry. The Am cutaneous penetration to the receiver compartment is almost negligible in fresh and frozen skin. Multiple washings with water and DTPA recovered about 90% of the initial activity. The rest remains fixed mainly in the stratum corneum. Traces of activity were detected within the epidermis and dermis which is fixed and not accessible to the decontamination. Copyright © 2016 Elsevier Ireland Ltd. All rights reserved.

Impact of Reprocessed Uranium Management on the Homogeneous Recycling of Transuranics in PWRs

DOE Office of Scientific and Technical Information (OSTI.GOV)

Youinou, Gilles J.

This article presents the results of a neutronics analysis related to the homogeneous recycling of transuranics (TRU) in PWRs with a MOX fuel using enriched uranium instead of depleted uranium. It also addresses an often, if not always, overlooked aspect related to the recycling of TRU in PWRs, namely the use of reprocessed uranium. From a neutronics point of view, it is possible to multi-recycle the entirety of the plutonium with or without neptunium and americium in a PWR fleet using MOX-EU fuel in between one third and two thirds of the fleet. Recycling neptunium and americium with plutonium significantlymore » decreases the decay heat of the waste stream between 100 to 1,000 years compared to those of an open fuel cycle or when only plutonium is recycled. The uranium present in MOX-EU used fuel still contains a significant amount of 235uranium and recycling it makes a major difference on the natural uranium needs. For example, a PWR fleet recycling its plutonium, neptunium and americium in MOXEU needs 28 percent more natural uranium than a reference UO 2 open cycle fleet generating the same energy if the reprocessed uranium is not recycled and 19 percent less if the reprocessed uranium is recycled back in the reactors, i.e. a 47 percent difference.« less

Impact of Reprocessed Uranium Management on the Homogeneous Recycling of Transuranics in PWRs

DOE PAGES

Youinou, Gilles J.

2017-05-04

This article presents the results of a neutronics analysis related to the homogeneous recycling of transuranics (TRU) in PWRs with a MOX fuel using enriched uranium instead of depleted uranium. It also addresses an often, if not always, overlooked aspect related to the recycling of TRU in PWRs, namely the use of reprocessed uranium. From a neutronics point of view, it is possible to multi-recycle the entirety of the plutonium with or without neptunium and americium in a PWR fleet using MOX-EU fuel in between one third and two thirds of the fleet. Recycling neptunium and americium with plutonium significantlymore » decreases the decay heat of the waste stream between 100 to 1,000 years compared to those of an open fuel cycle or when only plutonium is recycled. The uranium present in MOX-EU used fuel still contains a significant amount of 235uranium and recycling it makes a major difference on the natural uranium needs. For example, a PWR fleet recycling its plutonium, neptunium and americium in MOXEU needs 28 percent more natural uranium than a reference UO 2 open cycle fleet generating the same energy if the reprocessed uranium is not recycled and 19 percent less if the reprocessed uranium is recycled back in the reactors, i.e. a 47 percent difference.« less

Transfer of environmental plutonium and americium across the human gut.

PubMed

Hunt, G J; Leonard, D R; Lovett, M B

1986-08-01

Data on gut transfer factors for environmental forms of radionuclides are essential for estimates of public radiation exposures following ingestion, and thus in decisions on controlling waste discharges. Dose estimates for transuranic nuclides are particularly sensitive to uncertainties stemming from gut transfer data being related to non-environmental forms and/or derived from animal experiments. We have measured human gut transfer factors for plutonium and americium in two experiments using marine foods obtained near Sellafield, Cumbria. Firstly, the urine of volunteer members of the critical group of shellfish consumers was analysed for transuranics and the results related to their consumption rates. Secondly, remotely-based volunteers ate single quantities of shellfish obtained near Sellafield, and their urine was analysed. An overall result for the gut transfer factor for environmental plutonium of 0.8 X 10(-4) indicates no need to increase the value of 1 X 10(-4), currently used by the International Commission on Radiological Protection (ICRP) for soluble forms. Results for americium show that the ICRP value of 5 X 10(-4) is maximising, and that a value of 1 X 10(-4) would be supportable. The results from the study of critical group members provide confidence in our habits survey techniques and reassurance that there are no significant pathways for intake of transuranics by these people that have not been recognised.

Complete recovery of actinides from UREX-like raffinates using a combination of hard and soft donor ligands. II. soft donor structure variation

DOE PAGES

Zalupski, Peter R.; Klaehn, John R.; Peterman, Dean R.

2015-07-30

The feasibility of simultaneous separation of uranium, neptunium, plutonium, americium, and curium from a simulated dissolved used fuel simulant adjusted to 1.0 M nitric acid is investigated using a mixture of the soft donor bis(bis-3,5-trifluoromethyl)phenyl) dithiophosphinic acid (“0”) and the hard donor synergist trioctylphosphine oxide (TOPO) dissolved in toluene. The results reported in this work are compared to our recent demonstration of a complete actinide recovery from a simulated dissolved fuel solution using a synergistic combination of bis(o-trifluoromethylphenyl)dithiophosphinic acid (“1”) and TOPO dissolved in either toluene or trifluoromethylphenyl sulfone. While the extraction efficiency of americium was enhanced for the liquid-liquidmore » system containing “0”, enabling to accomplish a trivalent An/Ln separation at 1.0 M HNO3, the extraction of neptunium was drastically diminished, relative to “1”. The partitioning behavior of curium was also negatively impacted, introducing an effective opportunity for americium/curium separation. Radiometric and spectrophotometric studies demonstrate that the complete actinide recovery using the solvent based upon “0” and TOPO is not feasible. Additionally, the importance of radiolytic degradation processes is discussed through the comparisons of extraction properties of liquid-liquid systems based on both soft donor reagents.« less

Thermodynamic, Spectroscopic, and Computational Studies of f -Element Complexation by N -Hydroxyethyl-diethylenetriamine- N,N ', N ", N"-tetraacetic Acid

DOE Office of Scientific and Technical Information (OSTI.GOV)

Grimes, Travis S.; Heathman, Colt R.; Jansone-Popova, Santa

Potentiometric and spectroscopic techniques were combined with DFT calculations to probe the coordination environment and determine thermodynamic features of trivalent f-element complexation by N-hydroxyethyl-diethylenetriamine-N,N',N",N"-tetraacetic acid, HEDTTA. Ligand protonation constants and lanthanide stability constants were determined using potentiometry. Five protonation constants were accessible in I = 2.0 M (H +/Na +)ClO 4. UV–vis spectroscopy was used to determine stability constants for Nd 3+ and Am 3+ complexation with HEDTTA. Luminescence spectroscopy indicates two water molecules in the inner coordination sphere of the Eu/HEDTTA complex, suggesting HEDTTA is heptadentate. Luminescence data was supported by DFT calculations, which demonstrate that substitution of themore » acetate pendant arm by a N-hydroxyethyl group weakens the metal–nitrogen bond. This bond elongation is reflected in HEDTTA’s ability to differentiate trivalent actinides from trivalent lanthanides. The trans-lanthanide Ln/HEDTTA complex stability trend is analogous to Ln/DTPA complexation; however, the loss of one chelate ring resulting from structural substitution weakens the complexation by ~3 orders of magnitude. Successful separation of trivalent americium from trivalent lanthanides was demonstrated when HEDTTA was utilized as aqueous holdback complexant in a liquid–liquid system. Time-dependent extraction studies for HEDTTA were compared to diethylenetriamine-N,N,N',N",N"-pentaacetic acid (DTPA) and N-hydroxyethyl-ethylenediamine-N,N',N'-triacetic acid (HEDTA). The results presented here indicate substantially enhanced phase-transfer kinetic rates for mixtures containing HEDTTA.« less

Thermodynamic, Spectroscopic, and Computational Studies of f -Element Complexation by N -Hydroxyethyl-diethylenetriamine- N,N ', N ", N"-tetraacetic Acid

DOE PAGES

Grimes, Travis S.; Heathman, Colt R.; Jansone-Popova, Santa; ...

2017-01-24

Potentiometric and spectroscopic techniques were combined with DFT calculations to probe the coordination environment and determine thermodynamic features of trivalent f-element complexation by N-hydroxyethyl-diethylenetriamine-N,N',N",N"-tetraacetic acid, HEDTTA. Ligand protonation constants and lanthanide stability constants were determined using potentiometry. Five protonation constants were accessible in I = 2.0 M (H +/Na +)ClO 4. UV–vis spectroscopy was used to determine stability constants for Nd 3+ and Am 3+ complexation with HEDTTA. Luminescence spectroscopy indicates two water molecules in the inner coordination sphere of the Eu/HEDTTA complex, suggesting HEDTTA is heptadentate. Luminescence data was supported by DFT calculations, which demonstrate that substitution of themore » acetate pendant arm by a N-hydroxyethyl group weakens the metal–nitrogen bond. This bond elongation is reflected in HEDTTA’s ability to differentiate trivalent actinides from trivalent lanthanides. The trans-lanthanide Ln/HEDTTA complex stability trend is analogous to Ln/DTPA complexation; however, the loss of one chelate ring resulting from structural substitution weakens the complexation by ~3 orders of magnitude. Successful separation of trivalent americium from trivalent lanthanides was demonstrated when HEDTTA was utilized as aqueous holdback complexant in a liquid–liquid system. Time-dependent extraction studies for HEDTTA were compared to diethylenetriamine-N,N,N',N",N"-pentaacetic acid (DTPA) and N-hydroxyethyl-ethylenediamine-N,N',N'-triacetic acid (HEDTA). The results presented here indicate substantially enhanced phase-transfer kinetic rates for mixtures containing HEDTTA.« less

Summary report for the FY-2015 SACSESS Collaboration

DOE Office of Scientific and Technical Information (OSTI.GOV)

Peterman, Dean Richard; Mincher, Bruce Jay

2015-09-01

During FY-2015, a collaborative research program was established by the Department of Energy-Nuclear Energy (DOE-NE) Material Recovery and Waste Form Development program and the European Union (EU) Safety of Actinide Separation Processes (SACSESS) program. One component of this collaboration was the evaluation of the radiolytic stability of a Selective ActiNide Extraction (SANEX) separation which utilized a TODGA-based organic solvent and an aqueous phase containing the hydrophilic complexing reagent, SO3-Ph-BTP. To best simulate process conditions, this experiment was irradiated in the radiolysis/hydrolysis test loop located at the Idaho National Laboratory. The effect of irradiation on a SACSESS program iSANEX formulation containingmore » a TODGA-based organic phase and a BTP-based aqueous phase was investigated using irradiations at INL in static and test loop modes. When irradiated in contact with only the acidic aqueous phase, the TODGA organic solution maintained excellent extraction performance of americium, cerium and europium to a maximum absorbed dose of nearly 0.9 MGy. When the aqueous phase was changed to that containing the aqueous soluble BTP, the irradiated aqueous phase showed a dramatic color change, but this does not appear to have adverse effects on solvent extraction performance. Only minor increases in distribution ratios for both the lanthanides and actinide were measured, and the separation factors were essentially unchanged to a maximum absorbed dose of 174 kGy. The determination of the americium, cerium, and europium distribution ratios for the remaining SACSESS test loop samples will be completed in the near future. The analysis of stable metals concentration in the the irradiated aqueous and organic phases will be completed shortly.« less

Siderocalin-mediated recognition, sensitization, and cellular uptake of actinides.

PubMed

Allred, Benjamin E; Rupert, Peter B; Gauny, Stacey S; An, Dahlia D; Ralston, Corie Y; Sturzbecher-Hoehne, Manuel; Strong, Roland K; Abergel, Rebecca J

2015-08-18

Synthetic radionuclides, such as the transuranic actinides plutonium, americium, and curium, present severe health threats as contaminants, and understanding the scope of the biochemical interactions involved in actinide transport is instrumental in managing human contamination. Here we show that siderocalin, a mammalian siderophore-binding protein from the lipocalin family, specifically binds lanthanide and actinide complexes through molecular recognition of the ligands chelating the metal ions. Using crystallography, we structurally characterized the resulting siderocalin-transuranic actinide complexes, providing unprecedented insights into the biological coordination of heavy radioelements. In controlled in vitro assays, we found that intracellular plutonium uptake can occur through siderocalin-mediated endocytosis. We also demonstrated that siderocalin can act as a synergistic antenna to sensitize the luminescence of trivalent lanthanide and actinide ions in ternary protein-ligand complexes, dramatically increasing the brightness and efficiency of intramolecular energy transfer processes that give rise to metal luminescence. Our results identify siderocalin as a potential player in the biological trafficking of f elements, but through a secondary ligand-based metal sequestration mechanism. Beyond elucidating contamination pathways, this work is a starting point for the design of two-stage biomimetic platforms for photoluminescence, separation, and transport applications.

Siderocalin-mediated recognition, sensitization, and cellular uptake of actinides

PubMed Central

Allred, Benjamin E.; Rupert, Peter B.; Gauny, Stacey S.; An, Dahlia D.; Ralston, Corie Y.; Sturzbecher-Hoehne, Manuel; Strong, Roland K.; Abergel, Rebecca J.

2015-01-01

Synthetic radionuclides, such as the transuranic actinides plutonium, americium, and curium, present severe health threats as contaminants, and understanding the scope of the biochemical interactions involved in actinide transport is instrumental in managing human contamination. Here we show that siderocalin, a mammalian siderophore-binding protein from the lipocalin family, specifically binds lanthanide and actinide complexes through molecular recognition of the ligands chelating the metal ions. Using crystallography, we structurally characterized the resulting siderocalin–transuranic actinide complexes, providing unprecedented insights into the biological coordination of heavy radioelements. In controlled in vitro assays, we found that intracellular plutonium uptake can occur through siderocalin-mediated endocytosis. We also demonstrated that siderocalin can act as a synergistic antenna to sensitize the luminescence of trivalent lanthanide and actinide ions in ternary protein–ligand complexes, dramatically increasing the brightness and efficiency of intramolecular energy transfer processes that give rise to metal luminescence. Our results identify siderocalin as a potential player in the biological trafficking of f elements, but through a secondary ligand-based metal sequestration mechanism. Beyond elucidating contamination pathways, this work is a starting point for the design of two-stage biomimetic platforms for photoluminescence, separation, and transport applications. PMID:26240330

XRD monitoring of α self-irradiation in uranium-americium mixed oxides.

PubMed

Horlait, Denis; Lebreton, Florent; Roussel, Pascal; Delahaye, Thibaud

2013-12-16

The structural evolution under (241)Am self-irradiation of U(1-x)Am(x)O(2±δ) transmutation fuels (with x ≤ 0.5) was studied by X-ray diffraction (XRD). Samples first underwent a preliminary heat treatment performed under a reducing atmosphere (Ar/H2(4%)) aiming to recover the previously accumulated structural defects. Over all measurements (carried out over up to a full year and for integrated doses up to 1.5 × 10(18) α-decay events·g(-1)), only fluorite U(1-x)Am(x)O(2±δ) solid solutions were observed. Within a few days after the end of the heat treatment, each of the five studied samples was slowly oxidized as a consequence of their move to air atmosphere, which is evidenced by XRD by an initial sharp decrease of the unit cell parameter. For the compounds with x ≤ 0.15, this oxidation occurred without any phase transitions, but for U0.6Am0.4O(2±δ) and U0.5Am0.5O(2±δ), this process is accompanied by a transition from a first fluorite solid solution to a second oxidized one, as the latter is thermodynamically stable in ambient conditions. In the meantime and after the oxidation process, (241)Am α self-irradiation caused a structural swelling up to ∼0.8 vol %, independently of the sample composition. The kinetic constants of swelling were also determined by regression of experimental data and are, as expected, dependent on x and thus on the dose rate. The normalization of these kinetic constants by sample α-activity, however, leads to very close swelling rates among the samples. Finally, evolutions of microstrain and crystallite size were also monitored, but for the considered dose rates and cumulated doses, α self-irradiation was found, within the limits of the diffractometer used, to have almost no impact on these characteristics. Microstrain was found to be influenced instead by the americium content in the materials (i.e., by the impurities associated with americium starting material and the increase of cationic charge heterogeneity with increasing americium content).

Adsorption and Dissociation of Molecular Hydrogen on the (0001) Surface of DHCP Americium

NASA Astrophysics Data System (ADS)

Dholabhai, Pratik; Ray, Asok

2009-03-01

Hydrogen molecule adsorption on the (0001) surface of double hexagonal closed packed americium has been studied in detail within the framework of density functional theory. Weak molecular hydrogen adsorptions were observed. The most stable configuration corresponded to a Hor2 approach molecular adsorption at the one-fold top site where the molecule's approach is perpendicular to a lattice vector. Adsorption energies and adsorption geometries for different adsorption sites will be discussed. The change in work functions, magnetic moments, partial charges inside muffin-tins, difference charge density distributions and density of states for the bare Am slab and the Am slab after adsorption of the hydrogen molecule will be discussed. Reaction barrier for the dissociation of hydrogen molecule will be presented. The implications of adsorption on Am 5f electron localization-delocalization will be summarized.

Biodynamic study of americium-241 accumulation in the cytosol of the hepatopancreas of the lobster Homarus gammarus.

PubMed

Goudard, F; Paquet, F; Durand, J P; Milcent, M C; Germain, P; Pieri, J

1994-08-01

In the lobster, most of the radionuclides ingested with contaminated food are concentrated in the digestive gland. Americium-241 accumulation in the hepatopancreas of the lobster was studied during the digestive cycle. Fractionations of cytosols at different times after ingestion of radioactive preys were performed by gel permeation chromatography to determine the distribution of 241Am in the different macromolecular components. 241Am was associated with ferritin during the whole digestive cycle. This observation suggests a correlation between 241Am distribution pathways and iron metabolism. The distribution of 241Am present in the other cytosolic proteins followed two major steps of accumulation which may be correlated to the evolution of the two main cellular types playing an important role in the digestive cycle (B and R type cells).

Adsorption and Dissociation of Water on the (0001) Surface of DHCP Americium

NASA Astrophysics Data System (ADS)

Dholabhai, Pratik; Ray, Asok

2009-03-01

Ab initio total energy calculations within the framework of density functional theory have been performed for water molecule adsorption on the (0001) surface of double hexagonal closed packed americium. Subsequent partial dissociation (OH+H) and complete dissociation (H+O+H) of the water molecule have been examined. The completely dissociated configuration exhibits the strongest binding with the surface followed by partially dissociated species, with all molecular H2O configurations showing weak physisorption. The change in work functions and net magnetic moments before and after adsorption will be presented for all the cases studied. The adsorbate-substrate interactions will be elaborated using the difference charge density distributions and the local density of states. The effects of adsorption on Am 5f electron localization-delocalization in the vicinity of the Fermi level will be discussed.

Technical Improvements to an Absorbing Supergel for Radiological Decontamination in Tropical Environments

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kaminski, Michael D.; Mertz, Carol J.; Kivenas, Nadia

Argonne National Laboratory (Argonne) developed a superabsorbing gel-based process (SuperGel) for the decontamination of cesium from concrete and other porous building materials. Here, we report on results that tested the gel decontamination technology on specific concrete and ceramic formulations from a coastal city in Southeast Asia, which may differ significantly from some U.S. sources. Results are given for the evaluation of americium and cesium sequestering agents that are commercially available at a reasonable cost; the evaluation of a new SuperGel formulation that combines the decontamination properties of cesium and americium; the variation of the contamination concentration to determine the effectsmore » on the decontamination factors with concrete, tile, and brick samples; and pilot-scale testing (0.02–0.09 m2 or 6–12 in. square coupons).« less

In situ radiological surveying at the Double Tracks site, Nellis Air Force Range, Tonopah, Nevada

DOE Office of Scientific and Technical Information (OSTI.GOV)

Riedhauser, S.R.; Tipton, W.J.

1996-04-01

A team from the Remote Sensing Laboratory conducted a series of in situ radiological measurements at the Double Tracks site on the Nellis Air Force Range just east of Goldfield, Nevada, during the periods of April 10-13 and June 5-9, 1995. The survey team measured the terrestrial gamma radiation at the site to determine the levels of natural and man-made radiation. This site includes the areas covered by previous surveys conducted from 1962 through 1993. The main purpose of the first expedition was to assess several new techniques for characterizing sites with dispersed plutonium. The two purposes of the secondmore » expedition were to characterize the distribution of transuranic contamination (primarily plutonium) at the site by measuring the gamma rays from americium-241 and to assess the performance of the two new detector platforms. Both of the new platforms performed well, and the characterization of the americium-241 activity at the site was completed. Several plots compare these ground-based system measurements and the 1993 aerial data. The agreement is good considering the systems are characterized and calibrated through independent means. During the April expedition, several methods for measuring the depth distribution of americium-241 in the field were conducted as a way of quickly and reliably obtaining depth profiles without the need to wait for laboratory analysis. Two of the methods were not very effective, but the results of the third method appear very promising.« less

Evaluation of americium-241 toxicity influence on the microbial growth of organic wastes

DOE Office of Scientific and Technical Information (OSTI.GOV)

Takehiro Marumo, Julio; Padua Ferreira, Rafael Vicente de; Keiko Isiki, Vera Lucia

2007-07-01

Available in abstract form only. Full text of publication follows: Since the licenses for using radioactive sources in radioactive lightning rods were lifted by the Brazilian national nuclear authority, in 1989, the radioactive devices have been replaced by Franklin type and collected as radioactive waste. However, only 20 percent of the estimated total number of installed rods was delivered to Brazilian Nuclear Commission. This situation causes concern, due to, first, the possibility of the rods being disposed as domestic waste, and second, the americium, the most commonly employed radionuclide, is classified as a high-toxicity element. In the present study, Am-241more » migration experiments were performed by a lysimeter system, in order to evaluate the risk of contamination caused by radioactive lightning rods disposed as a common solid waste. Besides the risk evaluation, it is important to know the mechanism of the Am-241 release or retention in waste as well as its influence in the waste decomposition processes. Many factors are involved, but microorganisms present in the waste play an important role in its degradation, which control the physical and chemical processes. The objective of this work was to evaluate the Am-241 influence on the microbial population by counting number of cells in lysimeters leachate. Preliminary results suggest that americium may influence significantly the bacteria growth in organic waste, evidenced by culture under aerobiosis and an-aerobiosis and the antimicrobial resistance test. (authors)« less

Neutron irradiation of Am-241 effectively produces curium

NASA Technical Reports Server (NTRS)

Anderson, R. W.; Milstead, J.; Stewart, D. C.

1967-01-01

Computer study was made on the production of multicurie amounts of highly alpha-active curium 242 from americium 241 irradiation. The information available includes curium 242 yields, curium composition, irradiation data, and production techniques and safeguards.

Radionuclide solubility and speciation studies for the Yucca Mountain site characterization project

DOE Office of Scientific and Technical Information (OSTI.GOV)

Nitsche, H.; Roberts, K.; Prussin, T.

1992-12-01

Yucca Mountain, Nevada, USA, is being investigated for its suitability as a potential site for a geologic nuclear waste repository. As part of the site characterization studies, actinide solubilities and speciations were studied at pH 6, 7, and 8.5 at 25{degrees}C in two different groundwaters from the vicinity of Yucca Mountain. The groundwaters differ substantially in total dissolved carbonate concentration, and to a lesser extent in ionic strength. In the waters with higher carbonate content, the solubilities of neptunium(V) decreased, whereas those americium(III) increased at 25{degrees}KC and decreased at 60{degrees}C. The solids formed were sodium neptunium carbonates and americium hydroxycarbonates.more » Plutonium solubilities did not significantly change with changing water composition because the solubility-controlling solids were mostly amorphous Pu(IV) polymers that contained only small amounts of carbonate.« less

Radionuclide solubility and speciation studies for the Yucca Mountain site characterization project

DOE Office of Scientific and Technical Information (OSTI.GOV)

Nitsche, H.; Roberts, K.; Prussin, T.

1993-12-31

Yucca Mountain, Nevada, U.S.A., is being investigated for its suitability as a potential site for a geologic nuclear waste repository. As part of the site characterization studies, actinide solubilities and speciations were studied at pH 6, 7, and 8.5 at 25{degrees} and 60{degrees}C in two different groundwaters from the vicinity of Yucca Mountain. The groundwaters differ substantially in total dissolved carbonate concentration, and to a lesser extent in ionic strength. In the waters with higher carbonate content, the solubilities of neptunium(V) decreased, whereas those of americium (III) increased at 25{degrees}C and decreased at 60{degrees}C. The solids formed were sodium neptuniummore » carbonates and americium hydroxycarbonates. Plutonium solubilities did not significantly change with changing water composition because the solubility-controlling solids were mostly amorphous Pu(IV) polymers that contained only small amounts of carbonate.« less

Adsorption and Dissociation of Molecular Oxygen on the (0001) Surface of Double Hexagonal Close Packed Americium

NASA Astrophysics Data System (ADS)

Dholabhai, Pratik; Atta-Fynn, Raymond; Ray, Asok

2008-03-01

Oxygen molecule adsorption on (0001) surface of double hexagonal packed americium has been studied in detail within the framework of density functional theory using a full-potential all-electron linearized augmented plane wave plus local orbitals method. The most stable configuration corresponded to molecular dissociation with the oxygen atoms occupying neighboring three-fold hollow h3 sites. Chemisorption energies and adsorption geometries for the adsorbed species, and change in work functions, magnetic moments, partial charges inside muffin-tins, difference charge density distributions and density of states for the bare Am slab and the Am slab after adsorption of the oxygen molecule will be discussed. The effects of chemisorption on Am 5f electron localization-delocalization in the vicinity of the Fermi level and the reaction barrier calculation for the dissociation of oxygen molecule to the most stable h3 sites will be discussed.

A Density Functional Study of Atomic Hydrogen and Oxygen Chemisorptions on the (0001) Surface of Double Hexagonal Close Packed Americium

NASA Astrophysics Data System (ADS)

Dholabhai, Pratik; Atta-Fynn, Raymond; Ray, Asok

2008-03-01

Ab initio total energy calculations within the framework of density functional theory have been performed for atomic hydrogen and oxygen chemisorptions on the (0001) surface of double hexagonal packed americium using a full-potential all-electron linearized augmented plane wave plus local orbitals (FLAPW+lo) method. The three-fold hollow hcp site was found to be the most stable site for H adsorption, while the two-fold bridge adsorption site was found to be the most stable site for O adsorption. Chemisorption energies and adsorption geometries for different adsorption sites will be discussed. The change in work functions, magnetic moments, partial charges inside muffin-tins, difference charge density distributions and density of states for the bare Am slab and the Am slab after adsorption of the adatom will be discussed. The implications of chemisorption on Am 5f electron localization-delocalization will also be discussed.

Effect of low-dose ionizing radiation on luminous marine bacteria: radiation hormesis and toxicity.

PubMed

Kudryasheva, N S; Rozhko, T V

2015-04-01

The paper summarizes studies of effects of alpha- and beta-emitting radionuclides (americium-241, uranium-235+238, and tritium) on marine microorganisms under conditions of chronic low-dose irradiation in aqueous media. Luminous marine bacteria were chosen as an example of these microorganisms; bioluminescent intensity was used as a tested physiological parameter. Non-linear dose-effect dependence was demonstrated. Three successive stages in the bioluminescent response to americium-241 and tritium were found: 1--absence of effects (stress recognition), 2--activation (adaptive response), and 3--inhibition (suppression of physiological function, i.e. radiation toxicity). The effects were attributed to radiation hormesis phenomenon. Biological role of reactive oxygen species, secondary products of the radioactive decay, is discussed. The study suggests an approach to evaluation of non-toxic and toxic stages under conditions of chronic radioactive exposure. Copyright © 2015 Elsevier Ltd. All rights reserved.

New hydrolytically stable solvent for Am/Eu separation in acidic media

DOE Office of Scientific and Technical Information (OSTI.GOV)

Smirnov, I.V.; Babain, V.A.; Chirkov, A.V.

Americium and europium extraction by synergistic mixture of 2,6-bis(1-aryl-1H-tetrazol-5-yl)pyridines (ATP) - chlorinated cobalt dicarbollide (CCD) in polar diluent s from HNO{sub 3} media was studied. Meta-nitro-benzo-trifluoride, phenyl-tri-fluoro-methyl sulfone and 1,2-dichloroethane were used as diluents. The effect of diluent, composition of aqueous phase and substituent nature in aryl ring of ATPs on the extraction efficiency and selectivity of americium and europium separation was investigated. At the optimal ratio of nATP:CCD 1:1 the Am - Eu separation factor exceeded 90. Extraction of {sup 85}Sr, {sup 137}Cs and {sup 133}Ba was investigated and it was found that the mixture nATP-CCD provided the separationmore » of Sr /Ba pair with a factor of 35. High resistance of 2,6-bisaryltetrazolyl pyridines to the action of nitric acid was demonstrated. (authors)« less

Frontiers of Chemistry for Americium and Curium

DOE R&D Accomplishments Database

Keller, O. L. Jr.

1984-01-01

The discoveries of americium and curium were made only after Seaborg had formulated his actinide concept in order to design the chemistry needed to separate them from irradiated /sup 239/Pu targets. Their discoveries thus furnished the first clear-cut evidence that the series exists and justified Seaborg`s bold assumption that even though Th and Pa appeared to presage a following 6d series, the pattern established by the periodic table after Cs and Ba would be repeated exactly after Fr and Ra. That is to say, a new 5f element rare earth series (the actinides) would follow Ac in the same way the 4f rare earth series (the lanthanides) follows La. The consequences of the resulting half-filled 5f/sup 7/ shell at Cm were originally presented by Seaborg as a test of his hypothesis. Recent research is outlined that substantiates Seaborg`s predictions in new and definitive ways.

Combining CMPO and HEH[EHP] for Separating Trivalent Lanthanides from the Transuranic Elements

DOE Office of Scientific and Technical Information (OSTI.GOV)

Braley, Jenifer C.; Lumetta, Gregg J.; Carter, Jennifer C.

2013-09-05

Combining octyl(phenyl)-N,N-diisobutyl-carbamoylmethylphosphine oxide (CMPO) and 2-ethylhexylphosphonic acid mono-2-ethylhexyl ester (HEH[EHP]) into a single process solvent for separating transuranic elements from liquid high-level waste is explored. The lanthanides and americium can be co-extracted from HNO3 into 0.2 mol/L CMPO + 1.0 mol/L HEH[EHP] in n-dodecane. The extraction is relatively insensitive to the HNO3 concentration within 0.1 to 5 mol/L HNO3. Americium can be selectively stripped from the CMPO/HEH[EHP] solvent into a citrate-buffered N-(2-hydroxyethyl)ethylenediaminetriacetic acid solution . Separation factors >14 can be achieved in the range pH 2.5 to 3.7, and the separation factors are relatively insensitive to pH, a major advantagemore » of this solvent formulation.« less

Hexavalent Americium recovery using Copper(III) periodate

DOE PAGES

McCann, Kevin; Brigham, Derek M.; Morrison, Samuel; ...

2016-10-31

Separation of americium from the lanthanides is considered one of the most difficult separation steps in closing the nuclear fuel cycle. One approach to this separation could involve oxidizing americium to the hexavalent state to form a linear dioxo cation while the lanthanides remain as trivalent ions. This work considers aqueous soluble Cu 3+ periodate as an oxidant under molar nitric acid conditions to separate hexavalent Am with diamyl amylphosphonate (DAAP) in n-dodecane. Initial studies assessed the kinetics of Cu 3+ periodate autoreduction in acidic media to aid in development of the solvent extraction system. Following characterization of the Cumore » 3+ periodate oxidant, solvent extraction studies optimized the recovery of Am from varied nitric acid media and in the presence of other fission product, or fission product surrogate, species. Short aqueous/organic contact times encouraged successful recovery of Am (distribution values as high as 2) from nitric acid media in the absence of redox active fission products. In the presence of a post-plutonium uranium redox extraction (post-PUREX) simulant aqueous feed, precipitation of tetravalent species (Ce, Ru, Zr) occurred and the distribution values of 241Am were suppressed, suggesting some oxidizing capacity of the Cu 3+ periodate is significantly consumed by other redox active metals in the simulant. Furthermore, the manuscript demonstrates Cu 3+ periodate as a potentially viable oxidant for Am oxidation and recovery and notes the consumption of oxidizing capacity observed in the presence of the post-PUREX simulant feed will need to be addressed for any approach seeking to oxidize Am for separations relevant to the nuclear fuel cycle.« less

Hexavalent Americium Recovery Using Copper(III) Periodate

DOE Office of Scientific and Technical Information (OSTI.GOV)

McCann, Kevin; Brigham, Derek M.; Morrison, Samuel

2016-11-21

Separation of americium from the lanthanides is considered one of the most difficult separation steps in closing the nuclear fuel cycle. One approach to this separation could involve oxidizing americium to the hexavalent state to form a linear dioxo cation while the lanthanides remain as trivalent ions. This work considers aqueous soluble Cu3+ periodate as an oxidant under molar nitric acid conditions to separate hexavalent Am with diamyl amylphosphonate (DAAP) in n-dodecane. Initial studies assessed the kinetics of Cu3+ periodate auto-reduction in acidic media to aid in development of the solvent extraction system. Following characterization of the Cu3+ periodate oxidant,more » solvent extraction studies optimized the recovery of Am from varied nitric acid media and in the presence of other fission product, or fission product surrogate, species. Short aqueous/organic contact times encouraged successful recovery of Am (distribution values as high as 2) from nitric acid media in the absence of redox active fission products. In the presence of a post-PUREX simulant aqueous feed, precipitation of tetravalent species (Ce, Ru, Zr) occurred and the distribution values of 241Am were suppressed, suggesting some oxidizing capacity of the Cu3+ periodate is significantly consumed by other redox active metals in the simulant. The manuscript demonstrates Cu3+ periodate as a potentially viable oxidant for Am oxidation and recovery and notes the consumption of oxidizing capacity observed in the presence of the post-PUREX simulant feed will need to be addressed for any approach seeking to oxidize Am for separations relevant to the nuclear fuel cycle.« less

High Purity Americium-241 for Fuel Cycle R&D Program

DOE Office of Scientific and Technical Information (OSTI.GOV)

Dr. Paul A. Lessing

2011-07-01

Previously the U.S. Department of Energy released Am-241 for various applications such as smoke detectors and Am-Be neutron sources for oil wells. At this date there is a shortage of usable, higher purity Am-241 in metal and oxide form available in the United States. Recently, the limited source of Am-241 has been from Russia with production being contracted to existing customers. The shortage has resulted in the price per gram rising dramatically over the last few years. DOE-NE currently has need for high purity Am-241 metal and oxide to fabricate fuel pellets for reactor testing in the Fuel Cycle R&Dmore » program. All the available high purity americium has been gathered from within the DOE system of laboratories. However, this is only a fraction of the projected needs of FCRD over the next 10 years. Therefore, FCR&D has proposed extraction and purification concepts to extract Am-241 from a mixed AmO2-PuO2 feedstock stored at the Savannah River Site. The most simple extraction system is based upon high temperature reduction using lanthanum metal with concurrent evaporation and condensation to produce high purity Am metal. Metallic americium has over a four order of magnitude higher vapor pressure than plutonium. Results from small-scale reduction experiments are presented. These results confirm thermodynamic predictions that at 1000 deg C metallic lanthanum reduces both PuO2 and AmO2. Faster kinetics are expected for temperatures up to about 1500 deg C.« less

Rapid Method for Sodium Hydroxide Fusion of Asphalt ...

EPA Pesticide Factsheets

Technical Brief--Addendum to Selected Analytical Methods (SAM) 2012 The method will be used for qualitative analysis of americium-241, plutonium-238, plutonium-239, radium-226, strontium-90, uranium-234, uranium-235 and uranium-238 in asphalt matrices samples.

Actinide halide complexes

DOEpatents

Avens, Larry R.; Zwick, Bill D.; Sattelberger, Alfred P.; Clark, David L.; Watkin, John G.

1992-01-01

A compound of the formula MX.sub.n L.sub.m wherein M is a metal atom selected from the group consisting of thorium, plutonium, neptunium or americium, X is a halide atom, n is an integer selected from the group of three or four, L is a coordinating ligand selected from the group consisting of aprotic Lewis bases having an oxygen-, nitrogen-, sulfur-, or phosphorus-donor, and m is an integer selected from the group of three or four for monodentate ligands or is the integer two for bidentate ligands, where the sum of n+m equals seven or eight for monodentate ligands or five or six for bidentate ligands, a compound of the formula MX.sub.n wherein M, X, and n are as previously defined, and a process of preparing such actinide metal compounds including admixing the actinide metal in an aprotic Lewis base as a coordinating solvent in the presence of a halogen-containing oxidant, are provided.

Chelation and stabilization of berkelium in oxidation state +IV

DOE Office of Scientific and Technical Information (OSTI.GOV)

Deblonde, Gauthier J. -P.; Sturzbecher-Hoehne, Manuel; Rupert, Peter B.

Berkelium (Bk) has been predicted to be the only transplutonium element able to exhibit both +III and +IV oxidation states in solution, but evidence of a stable oxidized Bk chelate has so far remained elusive. Here, in this work, we describe the stabilization of the heaviest 4+ ion of the periodic table, under mild aqueous conditions, using a siderophore derivative. The resulting Bk(IV) complex exhibits luminescence via sensitization through an intramolecular antenna effect. This neutral Bk(IV) coordination compound is not sequestered by the protein siderocalin - a mammalian metal transporter - in contrast to the negatively charged species obtained withmore » neighbouring trivalent actinides americium, curium and californium (Cf). The corresponding Cf(III)-ligand-protein ternary adduct was characterized by X-ray diffraction analysis. Finally, combined with theoretical predictions, these data add significant insight to the field of transplutonium chemistry, and may lead to innovative Bk separation and purification processes.« less

Chelation and stabilization of berkelium in oxidation state +IV

DOE PAGES

Deblonde, Gauthier J. -P.; Sturzbecher-Hoehne, Manuel; Rupert, Peter B.; ...

2017-04-10

Berkelium (Bk) has been predicted to be the only transplutonium element able to exhibit both +III and +IV oxidation states in solution, but evidence of a stable oxidized Bk chelate has so far remained elusive. Here, in this work, we describe the stabilization of the heaviest 4+ ion of the periodic table, under mild aqueous conditions, using a siderophore derivative. The resulting Bk(IV) complex exhibits luminescence via sensitization through an intramolecular antenna effect. This neutral Bk(IV) coordination compound is not sequestered by the protein siderocalin - a mammalian metal transporter - in contrast to the negatively charged species obtained withmore » neighbouring trivalent actinides americium, curium and californium (Cf). The corresponding Cf(III)-ligand-protein ternary adduct was characterized by X-ray diffraction analysis. Finally, combined with theoretical predictions, these data add significant insight to the field of transplutonium chemistry, and may lead to innovative Bk separation and purification processes.« less

Actinide halide complexes

DOEpatents

Avens, L.R.; Zwick, B.D.; Sattelberger, A.P.; Clark, D.L.; Watkin, J.G.

1992-11-24

A compound is described of the formula MX[sub n]L[sub m] wherein M is a metal atom selected from the group consisting of thorium, plutonium, neptunium or americium, X is a halide atom, n is an integer selected from the group of three or four, L is a coordinating ligand selected from the group consisting of aprotic Lewis bases having an oxygen-, nitrogen-, sulfur-, or phosphorus-donor, and m is an integer selected from the group of three or four for monodentate ligands or is the integer two for bidentate ligands, where the sum of n+m equals seven or eight for monodentate ligands or five or six for bidentate ligands. A compound of the formula MX[sub n] wherein M, X, and n are as previously defined, and a process of preparing such actinide metal compounds are described including admixing the actinide metal in an aprotic Lewis base as a coordinating solvent in the presence of a halogen-containing oxidant.

Transportability Class of Americium in K Basin Sludge under Ambient and Hydrothermal Processing Conditions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Delegard, Calvin H.; Schmitt, Bruce E.; Schmidt, Andrew J.

2006-08-01

This report establishes the technical bases for using a ''slow uptake'' instead of a ''moderate uptake'' transportability class for americium-241 (241Am) for the K Basin Sludge Treatment Project (STP) dose consequence analysis. Slow uptake classes are used for most uranium and plutonium oxides. A moderate uptake class has been used in prior STP analyses for 241Am based on the properties of separated 241Am and its associated oxide. However, when 241Am exists as an ingrown progeny (and as a small mass fraction) within plutonium mixtures, it is appropriate to assign transportability factors of the predominant plutonium mixtures (typically slow) to themore » Am241. It is argued that the transportability factor for 241Am in sludge likewise should be slow because it exists as a small mass fraction as the ingrown progeny within the uranium oxide in sludge. In this report, the transportability class assignment for 241Am is underpinned with radiochemical characterization data on K Basin sludge and with studies conducted with other irradiated fuel exposed to elevated temperatures and conditions similar to the STP. Key findings and conclusions from evaluation of the characterization data and published literature are summarized here. Plutonium and 241Am make up very small fractions of the uranium within the K Basin sludge matrix. Plutonium is present at about 1 atom per 500 atoms of uranium and 241Am at about 1 atom per 19000 of uranium. Plutonium and americium are found to remain with uranium in the solid phase in all of the {approx}60 samples taken and analyzed from various sources of K Basin sludge. The uranium-specific concentrations of plutonium and americium also remain approximately constant over a uranium concentration range (in the dry sludge solids) from 0.2 to 94 wt%, a factor of {approx}460. This invariability demonstrates that 241Am does not partition from the uranium or plutonium fraction for any characterized sludge matrix. Most of the K Basin sludge characterization data is derived spent nuclear fuel corroded within the K Basins at 10-15?C. The STP process will place water-laden sludges from the K Basin in process vessels at {approx}150-180 C. Therefore, published studies with other irradiated (uranium oxide) fuel were examined. From these studies, the affinity of plutonium and americium for uranium in irradiated UO2 also was demonstrated at hydrothermal conditions (150 C anoxic liquid water) approaching those proposed for the STP process and even for hydrothermal conditions outside of the STP operating envelope (e.g., 150 C oxic and 100 C oxic and anoxic liquid water). In summary, by demonstrating that the chemical and physical behavior of 241Am in the sludge matrix is similar to that of the predominant species (uranium and for the plutonium from which it originates), a technical basis is provided for using the slow uptake transportability factor for 241Am that is currently used for plutonium and uranium oxides. The change from moderate to slow uptake for 241Am could reduce the overall analyzed dose consequences for the STP by more than 30%.« less

Analysis of large soil samples for actinides

DOEpatents

Maxwell, III; Sherrod, L [Aiken, SC

2009-03-24

A method of analyzing relatively large soil samples for actinides by employing a separation process that includes cerium fluoride precipitation for removing the soil matrix and precipitates plutonium, americium, and curium with cerium and hydrofluoric acid followed by separating these actinides using chromatography cartridges.

The Impact of Time on Decorporation Efficacy After a "Dirty Bomb" Attack Studied by Simulation.

PubMed

Rump, A; Stricklin, D; Lamkowski, A; Eder, S; Abend, M; Port, M

2016-11-01

Background: In the case of a nuclear or radiological incident, there is a risk of external and internal contamination with radionuclides in addition to external irradiation. There is no consensus whether decorporation treatment should be initiated right away on spec or pending the results of internal dosimetry to determine the indication. Method: Based on biokinetic models for plutonium-239, americium-241 and cesium-137, the efficacy of a decorporation treatment using DTPA or Prussian blue was simulated depending on the initiation time and the duration of treatment for different invasion pathways and physicochemical properties of the inhaled compounds. Results: For the same level of radioactivity incorporated, the committed effective dose increases with the speed of the invasion process. The impact of the initiation time of a decorporation treatment is particularly important when the absorption of the radionuclide is fast. Even if started early after incorporation, the therapeutic efficacy is less for americium-241 or cesium-137 compared to plutonium-239. Therapeutic efficacy increases with treatment duration up to about 90 days for plutonium-239 and cesium-137, whereas a prolongation of the treatment over this limit may further enhance efficacy in the case of americium-241. Conclusion: In the case of a nuclear incident, several fractions with different but a priori unknown physicochemical properties may be inhaled. Thus, decorporation therapy should be started as soon as possible after the incorporation of the radionuclide(s), as a loss of efficacy caused by a delay of treatment initiation possibly cannot be compensated later on. Treatment should be pursued for several months. © Georg Thieme Verlag KG Stuttgart · New York.

15. VIEW OF LABORATORY EQUIPMENT IN THE BUILDING 771 ANALYTICAL ...

Library of Congress Historic Buildings Survey, Historic Engineering Record, Historic Landscapes Survey

15. VIEW OF LABORATORY EQUIPMENT IN THE BUILDING 771 ANALYTICAL LABORATORY. THE LAB ANALYZED SAMPLES FOR PLUTONIUM, AMERICIUM, URANIUM, NEPTUNIUM, AND OTHER RADIOACTIVE ISOTOPES. (9/25/62) - Rocky Flats Plant, Plutonium Recovery & Fabrication Facility, North-central section of plant, Golden, Jefferson County, CO

13. VIEW OF THE MOLTEN SALT EXTRACTION LINE. THE MOLTEN ...

Library of Congress Historic Buildings Survey, Historic Engineering Record, Historic Landscapes Survey

13. VIEW OF THE MOLTEN SALT EXTRACTION LINE. THE MOLTEN SALT EXTRACTION PROCESS WAS USED TO PURIFY PLUTONIUM BY REMOVING AMERICIUM, A DECAY BY-PRODUCT OF PLUTONIUM. (1/98) - Rocky Flats Plant, Plutonium Fabrication, Central section of Plant, Golden, Jefferson County, CO

UNDERSTANDING VARIATION IN PARTITION COEFFICIENT KD, VALUES, VOLUME III: AMERICIUM, ARSENIC, CURIUM, IODINE, NEPTUNIUM, RADIUM, AND TECHNETIUM

EPA Science Inventory

This report describes the conceptualization, measurement, and use of the partition (or distribution) coefficient, Kd, parameter, and the geochemical aqueous solution and sorbent properties that are most important in controlling adsorption/retardation behavior of selected contamin...

Solution speciation of plutonium and Americium at an Australian legacy radioactive waste disposal site.

PubMed

Ikeda-Ohno, Atsushi; Harrison, Jennifer J; Thiruvoth, Sangeeth; Wilsher, Kerry; Wong, Henri K Y; Johansen, Mathew P; Waite, T David; Payne, Timothy E

2014-09-02

During the 1960s, radioactive waste containing small amounts of plutonium (Pu) and americium (Am) was disposed in shallow trenches at the Little Forest Burial Ground (LFBG), located near the southern suburbs of Sydney, Australia. Because of periodic saturation and overflowing of the former disposal trenches, Pu and Am have been transferred from the buried wastes into the surrounding surface soils. The presence of readily detected amounts of Pu and Am in the trench waters provides a unique opportunity to study their aqueous speciation under environmentally relevant conditions. This study aims to comprehensively investigate the chemical speciation of Pu and Am in the trench water by combining fluoride coprecipitation, solvent extraction, particle size fractionation, and thermochemical modeling. The predominant oxidation states of dissolved Pu and Am species were found to be Pu(IV) and Am(III), and large proportions of both actinides (Pu, 97.7%; Am, 86.8%) were associated with mobile colloids in the submicron size range. On the basis of this information, possible management options are assessed.

The 1976 Hanford Americium Accident: Then and Now

DOE Office of Scientific and Technical Information (OSTI.GOV)

Carbaugh, Eugene H.

2013-10-02

The 1976 chemical explosion of an 241Am ion exchange column at a Hanford Site waste management facility resulted in the extreme contamination of a worker with 241Am, nitric acid and debris. The worker underwent medical treatment for acid burns, as well as wound debridement, extensive personal skin decontamination and long-term DTPA chelation therapy for decorporation of americium-241. Because of the contamination levels and prolonged decontamination efforts, care was provided for the first three months at the unique Emergency Decontamination Facility with gradual transition to the patient’s home occurring over another two months. The medical treatment, management, and dosimetry of themore » patient have been well documented in numerous reports and journal articles. The lessons learned with regard to patient treatment and effectiveness of therapy still form the underlying philosophy of treatment for contaminated injuries. Changes in infrastructure and facilities as well as societal expectations make for interesting speculation as to how responses might differ today.« less

Assessment of radiation doses from residential smoke detectors that contain americium-241

NASA Astrophysics Data System (ADS)

Odonnell, F. R.; Etnier, E. L.; Holton, G. A.; Travis, C. C.

1981-10-01

External dose equivalents and internal dose commitments were estimated for individuals and populations from annual distribution, use, and disposal of 10 million ionization chamber smoke detectors that contain 110 kBq americium-241 each. Under exposure scenarios developed for normal distribution, use, and disposal using the best available information, annual external dose equivalents to average individuals were estimated to range from 4 fSv to 20 nSv for total body and from 7 fSv to 40 nSv for bone. Internal dose commitments to individuals under post disposal scenarios were estimated to range from 0.006 to 80 micro-Sv (0.0006 to 8 mrem) to total body and from 0.06 to 800 micro-Sv to bone. The total collective dose (the sum of external dose equivalents and 50-year internal dose commitments) for all individuals involved with distribution, use, or disposal of 10 million smoke detectors was estimated to be about 0.38 person-Sv (38 person-rem) to total body and 00 ft squared.

Americium-241 in surface soil associated with the Hanford site and vicinity

DOE Office of Scientific and Technical Information (OSTI.GOV)

Price, K.R.; Gilbert, R.O.; Gano, K.A.

1981-05-01

Various kinds of surface soil samples were collected and analyzed for Americium-241 (/sup 241/Am) to examine the feasibility of improving soil sample data for the Hanford Surface Environmental Surveillance Program. Results do not indicate that a major improvement would occur if procedures were changed from the current practices. Conclusions from this study are somewhat tempered by the very low levels of /sup 241/Am (< 0.10 pCi/g dry weight) detected in surface soil samples and by the fact that statistical significance depended on the type of statistical tests used. In general, the average concentration of /sup 241/Am in soil crust (0more » to 1.0 cm deep) was greater than the corresponding subsurface layer (1.0 to 2.5 cm deep), and the average concentration of /sup 241/Am in some onsite samples collected near the PUREX facility was greater than comparable samples collected 60 km upwind at an offsite location.« less

Effect of americium-241 on luminous bacteria. Role of peroxides.

PubMed

Alexandrova, M; Rozhko, T; Vydryakova, G; Kudryasheva, N

2011-04-01

The effect of americium-241 ((241)Am), an alpha-emitting radionuclide of high specific activity, on luminous bacteria Photobacterium phosphoreum was studied. Traces of (241)Am in nutrient media (0.16-6.67 kBq/L) suppressed the growth of bacteria, but enhanced luminescence intensity and quantum yield at room temperature. Lower temperature (4 °C) increased the time of bacterial luminescence and revealed a stage of bioluminescence inhibition after 150 h of bioluminescence registration start. The role of conditions of exposure the bacterial cells to the (241)Am is discussed. The effect of (241)Am on luminous bacteria was attributed to peroxide compounds generated in water solutions as secondary products of radioactive decay. Increase of peroxide concentration in (241)Am solutions was demonstrated; and the similarity of (241)Am and hydrogen peroxide effects on bacterial luminescence was revealed. The study provides a scientific basis for elaboration of bioluminescence-based assay to monitor radiotoxicity of alpha-emitting radionuclides in aquatic solutions. Copyright © 2011 Elsevier Ltd. All rights reserved.

Osteosarcoma development following single inhalation exposure to americium-241 in beagle dogs.

PubMed

Gillett, N A; Hahn, F F; Mewhinney, J A; Muggenberg, B A

1985-10-01

Young, mature Beagle dogs underwent single inhalation exposure to respirable aerosols of 241AmO2 to determine the radiation dose distribution to tissues. The dogs were serially sacrificed to assess the clearance of 241Am from the lung, the rate of translocation to internal organs, the pattern of retention in the organs, and the rates and modes of excretion. Americium dioxide was relatively soluble in the lung, leading to the translocation of significant quantities of 241Am to bone and liver, thus delivering radiation doses to these tissues nearly equal to that received by the lung. Osteoblastic osteosarcomas developed in four dogs surviving more than 1000 days after exposure. Histologically, all of the osteosarcomas were associated with areas of radiation osteodystrophy characterized by bone infarction, peritrabecular new bone formation, marrow fibrosis, and microresorptive cavities. The retention and translocation of inhaled 241Am in dogs is similar to that of man, indicating that 241Am inhaled by humans may potentially result in significant risk of bone tumor development.

Americium-241 integral radiative capture cross section in over-moderated neutron spectrum from pile oscillator measurements in the Minerve reactor

NASA Astrophysics Data System (ADS)

Geslot, Benoit; Gruel, Adrien; Ros, Paul; Blaise, Patrick; Leconte, Pierre; Noguere, Gilles; Mathieu, Ludovic; Villamarin, David; Becares, Vicente; Plompen, Arjan; Kopecky, Stefan; Schillebeeckx, Peter

2017-09-01

An experimental program, called AMSTRAMGRAM, was recently conducted in the Minerve low power reactor operated by CEA Cadarache within the frame of the CHANDA initiative (Solving CHAllenges in Nuclear Data). Its aim was to measure the integral capture cross section of 241Am in the thermal domain. Motivation of this work is driven by large differences in this actinide thermal point reported by major nuclear data libraries. The AMSTRAMGRAM experiment, that made use of well characterized EC-JRC americium samples, was based on the oscillation technique commonly implemented in the Minerve reactor. First results are presented and discussed in this article. A preliminary calculation scheme was used to compare measured and calculated results. It is shown that this work confirms a bias previously observed with JEFF-3.1.1 (C/E-1 = -10.5 ± 2%). On the opposite, the experiment is in close agreement with 241Am thermal point reported in JEFF-3.2 (C/E-1 = 0.5 ± 2%).

NIST Calibration of a Neutron Spectrometer ROSPEC.

PubMed

Heimbach, Craig

2006-01-01

A neutron spectrometer was acquired for use in the measurement of National Institute of Standards and Technology neutron fields. The spectrometer included options for the measurement of low and high energy neutrons, for a total measurement range from 0.01 eV up to 17 MeV. The spectrometer was evaluated in calibration fields and was used to determine the neutron spectrum of an Americium-Beryllium neutron source. The calibration fields used included bare and moderated (252)Cf, monoenergetic neutron fields of 2.5 MeV and 14 MeV, and a thermal-neutron beam. Using the calibration values determined in this exercise, the spectrometer gives a good approximation of the neutron spectrum, and excellent values for neutron fluence, for all NIST calibration fields. The spectrometer also measured an Americium-Beryllium neutron field in a NIST exposure facility and determined the field quite well. The spectrometer measured scattering effects in neutron spectra which previously could be determined only by calculation or integral measurements.

Radiation detector spectrum simulator

DOEpatents

Wolf, Michael A.; Crowell, John M.

1987-01-01

A small battery operated nuclear spectrum simulator having a noise source nerates pulses with a Gaussian distribution of amplitudes. A switched dc bias circuit cooperating therewith generates several nominal amplitudes of such pulses and a spectral distribution of pulses that closely simulates the spectrum produced by a radiation source such as Americium 241.

Radiation detector spectrum simulator

DOEpatents

Wolf, M.A.; Crowell, J.M.

1985-04-09

A small battery operated nuclear spectrum simulator having a noise source generates pulses with a Gaussian distribution of amplitudes. A switched dc bias circuit cooperating therewith to generate several nominal amplitudes of such pulses and a spectral distribution of pulses that closely simulates the spectrum produced by a radiation source such as Americium 241.

Low-energy gamma ray inspection of brazed aluminum joints

NASA Technical Reports Server (NTRS)

Brown, J. A.

1967-01-01

Americium 241 serves as a suitable radioisotope /gamma ray source/ and exposure probe for radiographic inspection of brazed aluminum joints in areas of limited accessibility. The powdered isotope is contained in a sealed capsule mounted at the end of a spring-loaded pushrod in the probe assembly.

Pentavalent neptunyl ([OΞNpΞO] +) cation–cation interactions in aqueous/polar organic mixed-solvent media

DOE Office of Scientific and Technical Information (OSTI.GOV)

Burn, Adam G.; Martin, Leigh R.; Nash, Kenneth L.

Bonding interactions between polyvalent cations and oxo-anions are well known and characterized by predictably favorable Gibbs energies in solution-phase coordination chemistry. In contrast, interactions between ions of like charge are generally expected to be repulsive and strongly influenced by cation solvation. An exception to this instinctive rule is found in the existence of complexes resulting from interactions of pentavalent actinyl cations ([O≡An≡O] +) with selected polyvalent cations. Such cation–cation complexes have been known to exist since the 1960s, when they were first reported by Sullivan and co-workers. The weak actinyl cation–cation complex, resulting from a bonding interaction between a pentavalentmore » linear dioxo actinyl cation donor and hexavalent actinyl or trivalent/tetravalent metal cation acceptor, has been most commonly seen in media in which water activities are reduced, principally highly-salted aqueous media. Such interactions of pentavalent actinides are of relevance in ongoing research that focuses on advanced nuclear fuel processing systems based on the upper oxidation states of americium. This investigation focuses on exploring the thermodynamic stability of complexes between selected highly-charged metal cations (Al 3+, Sc 3+, Cr 3+, Fe 3+, In 3+ and UO 2+ 2) and the pentavalent neptunyl cation (NpO + 2, whose coordination chemistry is similar to that of AmO + 2 while exhibiting significantly greater oxidation state stability) in aqueous–polar organic mixed-solvents. As a result, the Gibbs energies for the cation–cation complexation reactions are correlated with general features of electrostatic bonding models; the NpO + 2 • Cr 3+ complex exhibits unexpectedly strong interactions that may indicate significant covalency in the cation–cation bonding interaction.« less

Pentavalent neptunyl ([OΞNpΞO] +) cation–cation interactions in aqueous/polar organic mixed-solvent media

DOE PAGES

Burn, Adam G.; Martin, Leigh R.; Nash, Kenneth L.

2017-06-17

Bonding interactions between polyvalent cations and oxo-anions are well known and characterized by predictably favorable Gibbs energies in solution-phase coordination chemistry. In contrast, interactions between ions of like charge are generally expected to be repulsive and strongly influenced by cation solvation. An exception to this instinctive rule is found in the existence of complexes resulting from interactions of pentavalent actinyl cations ([O≡An≡O] +) with selected polyvalent cations. Such cation–cation complexes have been known to exist since the 1960s, when they were first reported by Sullivan and co-workers. The weak actinyl cation–cation complex, resulting from a bonding interaction between a pentavalentmore » linear dioxo actinyl cation donor and hexavalent actinyl or trivalent/tetravalent metal cation acceptor, has been most commonly seen in media in which water activities are reduced, principally highly-salted aqueous media. Such interactions of pentavalent actinides are of relevance in ongoing research that focuses on advanced nuclear fuel processing systems based on the upper oxidation states of americium. This investigation focuses on exploring the thermodynamic stability of complexes between selected highly-charged metal cations (Al 3+, Sc 3+, Cr 3+, Fe 3+, In 3+ and UO 2+ 2) and the pentavalent neptunyl cation (NpO + 2, whose coordination chemistry is similar to that of AmO + 2 while exhibiting significantly greater oxidation state stability) in aqueous–polar organic mixed-solvents. As a result, the Gibbs energies for the cation–cation complexation reactions are correlated with general features of electrostatic bonding models; the NpO + 2 • Cr 3+ complex exhibits unexpectedly strong interactions that may indicate significant covalency in the cation–cation bonding interaction.« less

Higher Americium Oxidation State Research Roadmap

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mincher, Bruce J.; Law, Jack D.; Goff, George S.

2015-12-18

The partitioning of hexavalent Am from dissolved nuclear fuel requires the ability to efficiently oxidize Am(III) to Am(VI) and to maintain that oxidation state for a length of time sufficient to perform the separation. Several oxidants have been, or are being developed. Chemical oxidants include Ag-catalyzed ozone, Ag-catalyzed peroxydisulfate, Cu(III) periodate, and sodium bismuthate. Hexavalent americium has also now successfully been prepared by electrolysis, using functionalized electrodes. So-called auto-reduction rates of Am(VI) are sufficiently slow to allow for separations. However, for separations based on solvent extraction or ion exchange using organic resins, the high valence state must be maintained undermore » the reducing conditions of the organic phase contact, and a holding oxidant is probably necessary. Until now, only Cu(III) periodate and sodium bismuthate oxidation have been successfully combined with solvent extraction separations. Bismuthate oxidation provided the higher DAm, since it acts as its own holding oxidant, and a successful hot test using centrifugal contactors was performed. For the other oxidants, Ag-catalyzed peroxydisulfate will not oxidize americium in nitric acid concentrations above 0.3 M, and it is not being further investigated. Peroxydisulfate in the absence of Ag catalysis is being used to prepare Am(V) in ion exchange work, discussed below. Preliminary work with Ag-catalyzed ozone has been unsuccessful for extractions of Am(VI) from 6.5 M HNO3, and only one attempt at extraction, also from 6.5 M HNO3, using the electrolytic oxidation has been attempted. However, this high acid concentration was based on the highest Am extraction efficiency using the bismuthate oxidant; which is only sparingly soluble, and thus the oxidation yield is based on bismuthate solubility. Lower acid concentrations may be sufficient with alternative oxidants and work with Ag-ozone, Cu(III) and electrolysis is on-going. Two non-solvent-extraction separations are also under investigation. The first would separate Am(VI) by co-crystallization with uranium and the other oxidizable actinides as their nitrate salts. This novel idea has been successful in lab scale testing, and merits further investigation. Similarly, success has been achieved in separations using inorganic or hybrid ion exchange materials to sorb the lanthanides and actinides, while allowing pentavalent americium to elute. This is the only technique currently investigating Am(V), despite the advantages of this oxidation state with regard to its higher stability. The ultimate destination for this roadmap is to develop an americium separation that can be applied under process conditions, preferably affording a co-separation of the actinyl (VI) ions. Toward that end, emphasis is given here to selection of a solvent extraction flowsheet for testing in the INL centrifugal contactor hot test bed during FY16. A solvent extraction process will be tested mainly because solvent extraction separations of Am(VI) are relatively mature and the test bed currently exists in a configuration to support them. Thus, a major goal of FY16 is to select the oxidant/ligand combination to run such a test using the contactors. The only ligands under consideration are DAAP and DEHBA. This is not to say that ion exchange and co-crystallization techniques are unimportant. They merit continued investigation, but are not mature enough for hot test bed testing at this time.« less

Supercritical fluid extraction and separation of uranium from other actinides.

PubMed

Quach, Donna L; Mincher, Bruce J; Wai, Chien M

2014-06-15

The feasibility of separating U from nitric acid solutions of mixed actinides using tri-n-butylphosphate (TBP)-modified supercritical fluid carbon dioxide (sc-CO2) was investigated. The actinides U, Np, Pu, and Am were extracted into sc-CO2 modified with TBP from a range of nitric acid concentrations, in the absence of, or in the presence of, a number of traditional reducing and/or complexing agents to demonstrate the separation of these metals from U under sc-CO2 conditions. The separation of U from Pu using sc-CO2 was successful at nitric acid concentrations of less than 3M in the presence of acetohydroxamic acid (AHA) or oxalic acid (OA) to mitigate Pu extraction, and the separation of U from Np was successful at nitric acid concentrations of less than 1M in the presence of AHA, OA, or sodium nitrite to mitigate Np extraction. Americium was not well extracted under any condition studied. Copyright © 2014 Elsevier B.V. All rights reserved.

Rapid Method for Sodium Hydroxide Fusion of Asphalt ...

EPA Pesticide Factsheets

Technical Brief--Addendum to Selected Analytical Methods (SAM) 2012 Rapid method developed for analysis of Americium-241 (241Am), plutonium-238 (238Pu), plutonium-239 (239Pu), radium-226 (226Ra), strontium-90 (90Sr), uranium-234 (234U), uranium-235 (235U) and uranium-238 (238U) in asphalt roofing material samples

Credibility of the threat from a radiological dispersal device by terrorists within the United States

DTIC Science & Technology

2016-06-10

on assessing the probability of an RDD attack, otherwise known as a “dirty bomb ,” within the US and its territories. Currently, there is an...officials arrested plotters planning to employ a dirty bomb utilizing americium obtained from smoke detectors.7 Officials thought it extremely unlikely

Comparative biokinetics of trivalent radionuclides with similar ionic dimensions: promethium-147, curium-242 and americium-241.

PubMed

Priest, N D

2007-09-01

Data on the distribution and redistribution patterns in the laboratory rat of three trivalent elements with a similar ionic radius have been compared. This showed that these distributions for the two ions with the same ionic radius (111 pm), i.e., those of promethium (a lanthanoid) and curium (an actinoid), were indistinguishable and that americium, with a slightly larger ion size (111.5 pm), behaved similarly. The results are consistent with the suggestion that ion size is the only important factor controlling the deposition and redistribution patterns of trivalent lanthanoids and actinoids in rats. The result is important because it suggests that the same radiological protection dosimetry models should be used for trivalent actinoids and lanthanoids, that human volunteer data generated for lanthanoid isotopes can be used to predict the behavior of actinoids with the same ion size, and that appropriate pairs of beta-particle-emitting lanthanoid and alpha-particle-emitting actinoids could be used to study the relative toxicity of alpha and beta particles in experimental animals.

Isotope ratio analysis of individual sub-micrometer plutonium particles with inductively coupled plasma mass spectrometry.

PubMed

Esaka, Fumitaka; Magara, Masaaki; Suzuki, Daisuke; Miyamoto, Yutaka; Lee, Chi-Gyu; Kimura, Takaumi

2010-12-15

Information on plutonium isotope ratios in individual particles is of great importance for nuclear safeguards, nuclear forensics and so on. Although secondary ion mass spectrometry (SIMS) is successfully utilized for the analysis of individual uranium particles, the isobaric interference of americium-241 to plutonium-241 makes difficult to obtain accurate isotope ratios in individual plutonium particles. In the present work, an analytical technique by a combination of chemical separation and inductively coupled plasma mass spectrometry (ICP-MS) is developed and applied to isotope ratio analysis of individual sub-micrometer plutonium particles. The ICP-MS results for individual plutonium particles prepared from a standard reference material (NBL SRM-947) indicate that the use of a desolvation system for sample introduction improves the precision of isotope ratios. In addition, the accuracy of the (241)Pu/(239)Pu isotope ratio is much improved, owing to the chemical separation of plutonium and americium. In conclusion, the performance of the proposed ICP-MS technique is sufficient for the analysis of individual plutonium particles. Copyright © 2010 Elsevier B.V. All rights reserved.

Assessment of radiation doses from residential smoke detectors that contain americium-241

DOE Office of Scientific and Technical Information (OSTI.GOV)

O'Donnell, F.R.; Etnier, E.L.; Holton, G.A.

1981-10-01

External dose equivalents and internal dose commitments were estimated for individuals and populations from annual distribution, use, and disposal of 10 million ionization chamber smoke detectors that contain 110 kBq (3 ..mu..Ci) americium-241 each. Under exposure scenarios developed for normal distribution, use, and disposal using the best available information, annual external dose equivalents to average individuals were estimated to range from 4 fSv (0.4 prem) to 20 nSv (2 ..mu..rem) for total body and from 7 fSv to 40 nSv for bone. Internal dose commitments to individuals under post disposal scenarios were estimated to range from 0.006 to 80 ..mu..Svmore » (0.0006 to 8 mrem) to total body and from 0.06 to 800 ..mu..Sv to bone. The total collective dose (the sum of external dose equivalents and 50-year internal dose commitments) for all individuals involved with distribution, use, or disposal of 10 million smoke detectors was estimated to be about 0.38 person-Sv (38 person-rem) to total body and 00 ft/sup 2/).« less

THERMODYNAMICS OF THE ACTINIDES

DOE Office of Scientific and Technical Information (OSTI.GOV)

Cunningham, Burris B.

1962-04-01

Recent work on the thermodynamic properties of the transplutonium elements is presented and discussed in relation to trends in thermodynamic properties of the actinide series. Accurate values are given for room temperature lattice parameters of two crystallographic forms, (facecentred cubic) fcc and dhcp (double-hexagonal closepacked), of americium metal and for the coefficients of thermal expansion between 157 and 878 deg K (dhcp) and 295 to 633 deg K (fcc). The meiting point of the metal, and its magnetic susceptibility between 77 and 823 deg K are reported and the latter compared with theoretical values for the tripositive ion calculated frommore » spectroscopic data. Similar data (crystallography, meiting point and magnetic susceptibility) are given for metallic curium. A value for the heat of formation of americium monoxide is reported in conjunction with crystallographic data on the monoxide and mononitride. A revision is made in the current value for the heat of formation of Am/O/sub 2/ and for the potential of the Am(III)-Am(IV) couple. The crystal structures and lattice parameters are reported for the trichloride, oxychloride and oxides of californium. (auth)« less

Americium characterization by X-ray fluorescence and absorption spectroscopy in plutonium uranium mixed oxide

NASA Astrophysics Data System (ADS)

Degueldre, Claude; Cozzo, Cedric; Martin, Matthias; Grolimund, Daniel; Mieszczynski, Cyprian

2013-06-01

Plutonium uranium mixed oxide (MOX) fuels are currently used in nuclear reactors. The actinides in these fuels need to be analyzed after irradiation for assessing their behaviour with regard to their environment and the coolant. In this work the study of the atomic structure and next-neighbour environment of Am in the (Pu,U)O2 lattice in an irradiated (60 MW d kg-1) MOX sample was performed employing micro-X-ray fluorescence (µ-XRF) and micro-X-ray absorption fine structure (µ-XAFS) spectroscopy. The chemical bonds, valences and stoichiometry of Am (˜0.66 wt%) are determined from the experimental data gained for the irradiated fuel material examined in its peripheral zone (rim) of the fuel. In the irradiated sample Am builds up as Am3+ species within an [AmO8]13- coordination environment (e.g. >90%) and no (<10%) Am(IV) or (V) can be detected in the rim zone. The occurrence of americium dioxide is avoided by the redox buffering activity of the uranium dioxide matrix.

In-situ X-ray diffraction study of phase transformations in the Am-O system

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lebreton, Florent, E-mail: florent.lebreton@cea.fr; GEMH, ENSCI, 87065 Limoges; Belin, Renaud C., E-mail: renaud.belin@cea.fr

2012-12-15

In the frame of minor actinides recycling, americium can be transmuted by adding it in UO{sub 2} or (U, Pu)O{sub 2} fuels. Americium oxides exhibiting a higher oxygen potential than U or Pu oxides, its addition alters the fuel properties. To comprehend its influence, a thorough knowledge of the Am-O phase equilibria diagram and of thermal expansion behavior is of main interest. Due to americium scarcity and high radiotoxicity, few experimental reports on this topic are available. Here we present in-situ high-temperature XRD results on the reduction from AmO{sub 2} to Am{sub 2}O{sub 3}. We show that fluorite (Fm-3m) AmO{submore » 2} is reduced to cubic (Ia-3) C Prime -type Am{sub 2}O{sub 3+{delta}}, and then into hexagonal (P6{sub 3}/mmc) A-type Am{sub 2}O{sub 3}, which remains stable up to 1840 K. We also demonstrate the transitional existence of the monoclinic (C2/m) B-type Am{sub 2}O{sub 3}. At last, we describe, for the first time, the thermal expansion behavior of the hexagonal Am{sub 2}O{sub 3} between room temperature and 1840 K. - Graphical abstract: Americium dioxide was in situ studied by high-temperature X-ray diffraction. First, fluorite AmO{sub 2} is reduced to cubic C Prime -type Am{sub 2}O{sub 3+{delta}} and then transforms into hexagonal A-type Am{sub 2}O{sub 3}, which remains stable up to 1840 K. Then, we demonstrate the transitional existence of monoclinic B-type Am{sub 2}O{sub 3}. At last, we describe, for the first time, the thermal expansion of A-type Am{sub 2}O{sub 3} between room temperature and 1840 K. This work may contribute to a better understanding of Am oxide behavior. Highlights: Black-Right-Pointing-Pointer We realize an in-situ high-temperature X-ray diffraction study on an AmO{sub 2} sample. Black-Right-Pointing-Pointer Fluorite AmO{sub 2} transforms to cubic Am{sub 2}O{sub 3+{delta}} and then to hexagonal Am{sub 2}O{sub 3}. Black-Right-Pointing-Pointer Little-known monoclinic Am{sub 2}O{sub 3} is observed during the cubic-to-hexagonal transition. Black-Right-Pointing-Pointer Lattice parameter thermal expansion of hexagonal Am{sub 2}O{sub 3} is given up to 1840 K. Black-Right-Pointing-Pointer We give additional data on AmO{sub 2} lattice parameter expansion under self-irradiation.« less

Historical review of californium-252 discovery and development

DOE Office of Scientific and Technical Information (OSTI.GOV)

Stoddard, D.H.

1985-01-01

This paper discusses the discovery and history of californium 252. This isotope may be synthesized by irradiating plutonium 239, plutonium 242, americium 243, or curium 244 with neutrons in a nuclear reactor. Various experiments and inventions involving /sup 252/Cf conducted at the Savannah River Plant are discussed. The evolution of radiotherapy using californium 252 is reviewed. (PLG)

10 CFR 32.102 - Schedule C-prototype tests for calibration or reference sources containing americium-241 or...

Code of Federal Regulations, 2012 CFR

2012-01-01

... entire radioactive surface of the source shall be wiped with filter paper, moistened with water, with the... wiped with filter paper with the application of moderate finger pressure. Removal of radioactive material from the source shall be determined by measuring the radioactivity on the filter paper or by...

Measuring soil moisture near soil surface...minor differences due to neutron source type

Treesearch

Robert R. Ziemer; Irving Goldberg; Norman A. MacGillivray

1967-01-01

Moisture measurements were made in three media?paraffin, water, saturated sand?with four neutron miusture meters, each containing 226-radium-beryllium, 227-actinium-beryllium, 238-plutonium-beryllium, or 241-americium-beryllium neutron sources. Variability in surface detection by the different sources may be due to differences in neutron sources, in length of source,...

Measuring soil moisture near soil surface ... minor differences due to neutron source type

Treesearch

Robert R. Ziemer; Irving Goldberg; Norman A. MacGillivray

1967-01-01

Abstract - Moisture measurements were made in three media--paraffin, water, saturated sand--with four neutron moisture meters, each containing 226-radium-beryllium, 227-actinium-beryllium, 239-plutonium-beryllium, or 241-americium-beryllium neutron sources. Variability in surface detection by the different sources may be due to differences in neutron sources, in...

A Novel Experiment to Investigate the Attenuation of Alpha Particles in Air

ERIC Educational Resources Information Center

Andrews, D. G. H.

2008-01-01

A simple student experiment investigating dependence on air pressure of the attenuation of alpha particles in air is described. An equation giving the pressure needed to absorb all alpha particles of a given energy is derived from the Bethe-Bloch formula. Results are presented for the attenuation of alpha particles from americium 241 and radium…

Historical Review of Californium-252 Discovery and Development

DOE R&D Accomplishments Database

Stoddard, D. H.

1985-01-01

This paper discusses the discovery and history of californium 252. This isotope may be synthesized by irradiating plutonium 239, plutonium 242, americium 243, or curium 244 with neutrons in a nuclear reactor. Various experiments and inventions involving Cf conducted at the Savannah River Plant are discussed. The evolution of radiotherapy using californium 252 is reviewed. (PLG)

10 CFR 32.102 - Schedule C-prototype tests for calibration or reference sources containing americium-241 or...

Code of Federal Regulations, 2010 CFR

2010-01-01

... 10 Energy 1 2010-01-01 2010-01-01 false Schedule C-prototype tests for calibration or reference... Licensed Items § 32.102 Schedule C—prototype tests for calibration or reference sources containing..., conduct prototype tests, in the order listed, on each of five prototypes of the source, which contains...

Monitored Natural Attenuation of Inorganic Contaminants in Ground Water Volume 3 Assessment for Radionuclides IncludingTritium, Radon, Strontium, Technetium, Uranium, Iodine, Radium, Thorium, Cesium, and Plutonium-Americium

EPA Science Inventory

The current document represents the third volume of a set of three volumes that address the technical basis and requirements for assessing the potential applicability of MNA as part of a ground-water remedy for plumes with nonradionuclide and/or radionuclide inorganic contamina...

Determining the dissolution rates of actinide glasses: A time and temperature Product Consistency Test study

DOE Office of Scientific and Technical Information (OSTI.GOV)

Daniel, W.E.; Best, D.R.

1995-12-01

Vitrification has been identified as one potential option for the e materials such as Americium (Am), Curium (Cm), Neptunium (Np), and Plutonium (Pu). A process is being developed at the Savannah River Site to safely vitrify all of the highly radioactive Am/Cm material and a portion of the fissile (Pu) actinide materials stored on site. Vitrification of the Am/Cm will allow the material to be transported and easily stored at the Oak Ridge National Laboratory. The Am/Cm glass has been specifically designed to be (1) highly durable in aqueous environments and (2) selectively attacked by nitric acid to allow recoverymore » of the valuable Am and Cm isotopes. A similar glass composition will allow for safe storage of surplus plutonium. This paper will address the composition, relative durability, and dissolution rate characteristics of the actinide glass, Loeffler Target, that will be used in the Americium/Curium Vitrification Project at Westinghouse Savannah River Company near Aiken, South Carolina. The first part discusses the tests performed on the Loeffler Target Glass concerning instantaneous dissolution rates. The second part presents information concerning pseudo-activation energy for the one week glass dissolution process.« less

Waste Isolation Pilot Plant Salt Decontamination Testing

DOE Office of Scientific and Technical Information (OSTI.GOV)

Demmer, Ricky Lynn; Reese, Stephen Joseph

2015-03-01

On February 14, 2014, americium and plutonium contamination was released in the Waste Isolation Pilot Plant (WIPP) salt caverns. Several practical, easily deployable methods of decontaminating WIPP salt, using a surrogate contaminant and americium (241Am), were developed and tested. The effectiveness of the methods is evaluated qualitatively, and to the extent practical, quantitatively. Of the methods tested (dry brushing, vacuum cleaning, water washing, mechanical grinding, strippable coatings, and fixative barriers), the most practical seems to be water washing. Effectiveness is very high, and water washing is easy and rapid to deploy. The amount of wastewater produced (~2 L/m2) would bemore » substantial and may not be easy to manage, but the method is the clear winner from a usability perspective. Removable surface contamination levels (smear results) from water washed coupons found no residual removable contamination. Thus, whatever contamination is left is likely adhered to (or trapped within) the salt. The other option that shows promise is the use of a fixative barrier. Bartlett Nuclear, Inc.’s Polymeric Barrier System proved the most durable of the coatings tested. The coatings were not tested for contaminant entrapment, only for coating integrity and durability.« less

Transuranic Contamination in Sediment and Groundwater at the U.S. DOE Hanford Site

DOE Office of Scientific and Technical Information (OSTI.GOV)

Cantrell, Kirk J.

2009-08-20

A review of transuranic radionuclide contamination in sediments and groundwater at the DOE’s Hanford Site was conducted. The review focused primarily on plutonium-239/240 and americium-241; however, other transuranic nuclides were discussed as well, including neptunium-237, plutonium-238, and plutonium-241. The scope of the review included liquid process wastes intentionally disposed to constructed waste disposal facilities such as trenches and cribs, burial grounds, and unplanned releases to the ground surface. The review did not include liquid wastes disposed to tanks or solid wastes disposed to burial grounds. It is estimated that over 11,800 Ci of plutonium-239, 28,700 Ci of americium-241, and 55more » Ci of neptunium-237 have been disposed as liquid waste to the near surface environment at the Hanford Site. Despite the very large quantities of transuranic contaminants disposed to the vadose zone at Hanford, only minuscule amounts have entered the groundwater. Currently, no wells onsite exceed the DOE derived concentration guide for plutonium-239/240 (30 pCi/L) or any other transuranic contaminant in filtered samples. The DOE derived concentration guide was exceeded by a small fraction in unfiltered samples from one well (299-E28-23) in recent years (35.4 and 40.4 pCi/L in FY 2006). The primary reason that disposal of these large quantities of transuranic radionuclides directly to the vadose zone at the Hanford Site has not resulted in widespread groundwater contamination is that under the typical oxidizing and neutral to slightly alkaline pH conditions of the Hanford vadose zone, transuranic radionuclides (plutonium and americium in particular) have a very low solubility and high affinity for surface adsorption to mineral surfaces common within the Hanford vadose zone. Other important factors are the fact that the vadose zone is typically very thick (hundreds of feet) and the net infiltration rate is very low due to the desert climate. In some cases where transuranic radionuclides have been co-disposed with acidic liquid waste, transport through the vadose zone for considerable distances has occurred. For example, at the 216-Z-9 Crib, plutonium-239 and americium-241 have moved to depths in excess of 36 m (118 ft) bgs. Acidic conditions increase the solubility of these contaminants and reduce adsorption to mineral surfaces. Subsequent neutralization of the acidity by naturally occurring calcite in the vadose zone (particularly in the Cold Creek unit) appears to have effectively stopped further migration. The vast majority of transuranic contaminants disposed to the vadose zone on the Hanford Site (10,200 Ci [86%] of plutonium-239; 27,900 Ci [97%] of americium-241; and 41.8 Ci [78%] of neptunium-237) were disposed in sites within the PFP Closure Zone. This closure zone is located within the 200 West Area (see Figures 1.1 and 3.1). Other closure zones with notably high quantities of transuranic contaminant disposal include the T Farm Zone with 408 Ci (3.5%) plutonium-239, the PUREX Zone with 330 Ci (2.8%) plutonium-239, 200-W Ponds Zone with 324 Ci (2.8%) plutonium-239, B Farm Zone with 183 Ci (1.6%) plutonium-239, and the REDOX Zone with 164 Ci (1.4%) plutonium 239. Characterization studies for most of the sites reviewed in the document are generally limited. The most prevalent characterization methods used were geophysical logging methods. Characterization of a number of sites included laboratory analysis of borehole sediment samples specifically for radionuclides and other contaminants, and geologic and hydrologic properties. In some instances, more detailed research level studies were conducted. Results of these studies were summarized in the document.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wilden, Andreas; Lumetta, Gregg J.; Sadowski, Fabian

A solvent extraction system has been developed for separating trivalent actinides from lanthanides. This “Advanced TALSPEAK” system uses 2-ethylhexylphosphonic acid mono-2-ethylhexyl ester to extract the lanthanides into a n-dodecane-based solvent phase, while the actinides are retained in a citrate-buffered aqueous phase by complexation to N-(2-hydroxyethyl)ethylenediamine-N,N',N'-triacetic acid. Batch distribution measurements indicate that the separation of americium from the light lanthanides decreases as the pH decreases. For example, the separation factor between La and Am increases from 2.5 at pH 2.0 to 19.3 at pH 3.0. However, previous investigations indicated that the extraction rates for the heavier lanthanides decrease with increasing pH.more » So, a balance between these two competing effects is required. An aqueous phase in which the pH was set at 2.6 was chosen for further process development because this offered optimal separation, with a minimum separation factor of ~8.4, based on the separation between La and Am. Centrifugal contactor single-stage efficiencies were measured to characterize the performance of the system under flow conditions.« less

Plutonium weathering on Johnston Atoll

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wolf, S.E.; Bates, J.K.; Buck, E.C.

1995-12-31

Johnston Atoll was contaminated with transuranic elements, particularly plutonium, by atmospheric nuclear weapons tests and aborted nuclear devices. Initial cleanup operations and and an extensive soil remediation program were performed. However, many areas contained a low-level continuum of activity, and subsurface contamination has been detected. Discrete hot particles and contaminated soil were characterized to determine whether the spread of activity was caused by weathering. Analytical techniques included gamma spectrometry, alpha spectrometry, and inductively coupled plasma-mass spectrometry to determine transuranic elemental and isotopic composition. Ultrafiltration and small-particle handling techniques were employed to isolate individual particles. Optical microscopy, scanning electron microscopy, analyticalmore » transmission electron microscopy, energy dispersive X-ray spectroscopy, and electron energy loss spectroscopy were used to characterize individual particles. Analyses of the hot particles showed that they are aborted nuclear warhead fragments that been melted and weathered in the presence of water and CaCO{sub 3}. It was concluded that the formation of aqueous ionic (Pu/Am)-CO{sub 3} coordinated complexes, during environmental exposure to large volumes of rainwater and carbonate-satured seawater, enhanced the solubility of transuranic elements. The (Pu/Am)-CO{sub 3} complexes sorbed onto colloidal CaCO{sub 3} and coral soil surfaces as they were exposed to rain and seawater. This mechanism led to greater dispersal of plutonium and americium than would be expected by physical transport of discrete hot particles alone.« less

Combined transuranic-strontium extraction process

DOEpatents

Horwitz, E.P.; Dietz, M.L.

1992-12-08

The transuranic (TRU) elements neptunium, plutonium and americium can be separated together with strontium from nitric acid waste solutions in a single process. An extractant solution of a crown ether and an alkyl(phenyl)-N,N-dialkylcarbanylmethylphosphine oxide in an appropriate diluent will extract the TRU's together with strontium, uranium and technetium. The TRU's and the strontium can then be selectively stripped from the extractant for disposal. 3 figs.

Combined transuranic-strontium extraction process

DOEpatents

Horwitz, E. Philip; Dietz, Mark L.

1992-01-01

The transuranic (TRU) elements neptunium, plutonium and americium can be separated together with strontium from nitric acid waste solutions in a single process. An extractant solution of a crown ether and an alkyl(phenyl)-N,N-dialkylcarbanylmethylphosphine oxide in an appropriate diluent will extract the TRU's together with strontium, uranium and technetium. The TRU's and the strontium can then be selectively stripped from the extractant for disposal.

Combined time-resolved laser fluorescence spectroscopy and extended X-ray absorption fine structure spectroscopy study on the complexation of trivalent actinides with chloride at T = 25-200 °C.

PubMed

Skerencak-Frech, Andrej; Fröhlich, Daniel R; Rothe, Jörg; Dardenne, Kathy; Panak, Petra J

2014-01-21

The complexation of trivalent actinides (An(III)) with chloride is studied in the temperature range from 25 to 200 °C by spectroscopic methods. Time-resolved laser fluorescence spectroscopy (TRLFS) is applied to determine the thermodynamic data of Cm(III)-Cl(-) complexes, while extended X-ray absorption fine structure spectroscopy (EXAFS) is used to determine the structural data of the respective Am(III) complexes. The experiments are performed in a custom-built high-temperature cell which is modified for the respective spectroscopic technique. The TRLFS results show that at 25 °C the speciation is dominated mainly by the Cm(3+) aquo ion. Only a minor fraction of the CmCl(2+) complex is present in solution. As the temperature increases, the fraction of this species decreases further. Simultaneously, the fraction of the CmCl2(+) complex increases strongly with the temperature. Also, the CmCl3 complex is formed to a minor extent at T > 160 °C. The conditional stability constant log β'2 is determined as a function of the temperature and extrapolated to zero ionic strength with the specific ion interaction theory approach. The log β°2(T) values increase by more than 3 orders of magnitude in the studied temperature range. The temperature dependency of log β°2 is fitted by the extended van't Hoff equation to determine ΔrH°m, ΔrS°m, and ΔrC°p,m. The EXAFS results support these findings. The results confirm the absence of americium(III) chloride complexes at T = 25 and 90 °C ([Am(III)] = 10(-3) m, [Cl(-)] = 3.0 m), and the spectra are described by 9-10 oxygen atoms at a distance of 2.44-2.48 Å. At T = 200 °C two chloride ligands are present in the inner coordination sphere of Am(III) at a distance of 2.78 Å.

Soil Sample Dissolution Development by Ultrawave Digester, Followed by Isotopic Separation and Analysis

DTIC Science & Technology

2017-01-09

uranium, americium, and thorium were analyzed, along with other transition and rare earth metals, utilizing inductively coupled plasma- mass spectrometry...inductively coupled plasma- mass spectrometry and/or alpha spectrometry, following digestion. For validation of the microwave protocol, radioactive... actinide elements. HF is a hazardous acid to work with and it is highly toxic. In this evaluation and validation, the actinides are of particular

Determination of actinides in urine and fecal samples

DOEpatents

McKibbin, Terry T.

1993-01-01

A method of determining the radioactivity of specific actinides that are carried in urine or fecal sample material is disclosed. The samples are ashed in a muffle furnace, dissolved in an acid, and then treated in a series of steps of reduction, oxidation, dissolution, and precipitation, including a unique step of passing a solution through a chloride form anion exchange resin for separation of uranium and plutonium from americium.

Determination of actinides in urine and fecal samples

DOEpatents

McKibbin, T.T.

1993-03-02

A method of determining the radioactivity of specific actinides that are carried in urine or fecal sample material is disclosed. The samples are ashed in a muffle furnace, dissolved in an acid, and then treated in a series of steps of reduction, oxidation, dissolution, and precipitation, including a unique step of passing a solution through a chloride form anion exchange resin for separation of uranium and plutonium from americium.

[The effect of the intratracheal administration of americium-241 on rat alveolar macrophages].

PubMed

Shopova, V; Sŭlovski, P; Dancheva, V

1996-01-01

In experiments in rats it was found that 241Am transitory decreases the total cell number and alveolar macrophage's percentage in bronchoalveolar lavage fluid (BALF): increases the macrophages size and nuclear size; and increases acid phosphatase and lactate dehydrogenase activities in BALF. It was suggested that 241Am causes and activation in the alveolar macrophages which probably appears as one of factors provoking lung injuries.

Americium-Curium Stabilization - 5'' Cylindrical Induction Melter System Design Basis

DOE Office of Scientific and Technical Information (OSTI.GOV)

Witt, D.C.

1999-11-08

Approximately 11,000 liters (3,600) gallons of solution containing isotopes of Am and Cm are currently stored in F-Canyon Tank 17.1. These isotopes were recovered during plutonium-242 production campaigns in the mid- and late-1970s. Experimental work for the project began in 1995 by the Savannah River Technology Center (SRTC). Details of the process are given in the various sections of this document.

Quantitative NDA measurements of advanced reprocessing product materials containing uranium, neptunium, plutonium, and americium

NASA Astrophysics Data System (ADS)

Goddard, Braden

The ability of inspection agencies and facility operators to measure powders containing several actinides is increasingly necessary as new reprocessing techniques and fuel forms are being developed. These powders are difficult to measure with nondestructive assay (NDA) techniques because neutrons emitted from induced and spontaneous fission of different nuclides are very similar. A neutron multiplicity technique based on first principle methods was developed to measure these powders by exploiting isotope-specific nuclear properties, such as the energy-dependent fission cross sections and the neutron induced fission neutron multiplicity. This technique was tested through extensive simulations using the Monte Carlo N-Particle eXtended (MCNPX) code and by one measurement campaign using the Active Well Coincidence Counter (AWCC) and two measurement campaigns using the Epithermal Neutron Multiplicity Counter (ENMC) with various (alpha,n) sources and actinide materials. Four potential applications of this first principle technique have been identified: (1) quantitative measurement of uranium, neptunium, plutonium, and americium materials; (2) quantitative measurement of mixed oxide (MOX) materials; (3) quantitative measurement of uranium materials; and (4) weapons verification in arms control agreements. This technique still has several challenges which need to be overcome, the largest of these being the challenge of having high-precision active and passive measurements to produce results with acceptably small uncertainties.

Measured solubilities and speciations of neptunium, plutonium, and americium in a typical groundwater (J-13) from the Yucca Mountain region; Milestone report 3010-WBS 1.2.3.4.1.3.1

DOE Office of Scientific and Technical Information (OSTI.GOV)

Nitsche, H.; Gatti, R.C.; Standifer, E.M.

1993-07-01

Solubility and speciation data are important in understanding aqueous radionuclide transport through the geosphere. They define the source term for transport retardation processes such as sorption and colloid formation. Solubility and speciation data are useful in verifying the validity of geochemical codes that are part of predictive transport models. Results are presented from solubility and speciation experiments of {sup 237}NpO{sub 2}{sup +}, {sup 239}Pu{sup 4+}, {sup 241}Am{sup 3+}/Nd{sup 3+}, and {sup 243}Am{sup 3+} in J-13 groundwater (from the Yucca Mountain region, Nevada, which is being investigated as a potential high-level nuclear waste disposal site) at three different temperatures (25{degree}, 60{degree},more » and 90{degree}C) and pH values (5.9, 7.0, and 8.5). The solubility-controlling steady-state solids were identified and the speciation and/or oxidation states present in the supernatant solutions were determined. The neptunium solubility decreased with increasing temperature and pH. Plutonium concentrations decreased with increasing temperature and showed no trend with pH. The americium solutions showed no clear solubility trend with increasing temperature and increasing pH.« less

Recent advances in f-element separations based on a new method for the production of pentavalent americium in acidic solution

DOE PAGES

Mincher, Bruce J.; Schmitt, Nicholas C.; Schuetz, Brian K.; ...

2015-03-11

The peroxydisulfate anion has long been used for the preparation of hexavalent americium (Am VI) from the normally stable Am III valence state in mildly acidic solutions. However, there has been no satisfactory means to directly prepare the pentavalent state (Am V) in that medium. Some early literature reports indicated that the peroxydisulfate oxidation was incomplete, and silver ion catalysis in conjunction with peroxydisulfate became accepted as the means to ensure quantitative generation of Am VI. Incomplete oxidation would be expected to leave residual Am III, or to produce Am V in treated solutions. However, until recently, the use ofmore » peroxydisulfate as an Am V reagent has not been reported. Here, parameters influencing the oxidation were investigated, including peroxydisulfate and acid concentration, temperature, duration of oxidative treatment, and the presence of higher concentrations of other redox active metals such as plutonium. Using optimized conditions determined here, quantitative Am V was prepared in an acidic solution and the UV/Vis extinction coefficients of the Am V 513 nm peak were measured over a range of nitric acid concentrations. Furthermore, the utility of Am V for separations from the lanthanides and curium by solvent extraction, organic column chromatography and inorganic ion exchangers was also investigated.« less

The design of a multisource americium-beryllium (Am-Be) neutron irradiation facility using MCNP for the neutronic performance calculation.

PubMed

Sogbadji, R B M; Abrefah, R G; Nyarko, B J B; Akaho, E H K; Odoi, H C; Attakorah-Birinkorang, S

2014-08-01

The americium-beryllium neutron irradiation facility at the National Nuclear Research Institute (NNRI), Ghana, was re-designed with four 20 Ci sources using Monte Carlo N-Particle (MCNP) code to investigate the maximum amount of flux that is produced by the combined sources. The results were compared with a single source Am-Be irradiation facility. The main objective was to enable us to harness the maximum amount of flux for the optimization of neutron activation analysis and to enable smaller sample sized samples to be irradiated. Using MCNP for the design construction and neutronic performance calculation, it was realized that the single-source Am-Be design produced a thermal neutron flux of (1.8±0.0007)×10(6) n/cm(2)s and the four-source Am-Be design produced a thermal neutron flux of (5.4±0.0007)×10(6) n/cm(2)s which is a factor of 3.5 fold increase compared to the single-source Am-Be design. The criticality effective, k(eff), of the single-source and the four-source Am-Be designs were found to be 0.00115±0.0008 and 0.00143±0.0008, respectively. Copyright © 2014 Elsevier Ltd. All rights reserved.

Characterization of neutron calibration fields at the TINT's 50 Ci americium-241/beryllium neutron irradiator

NASA Astrophysics Data System (ADS)

Liamsuwan, T.; Channuie, J.; Ratanatongchai, W.

2015-05-01

Reliable measurement of neutron radiation is important for monitoring and protection in workplace where neutrons are present. Although Thailand has been familiar with applications of neutron sources and neutron beams for many decades, there is no calibration facility dedicated to neutron measuring devices available in the country. Recently, Thailand Institute of Nuclear Technology (TINT) has set up a multi-purpose irradiation facility equipped with a 50 Ci americium-241/beryllium neutron irradiator. The facility is planned to be used for research, nuclear analytical techniques and, among other applications, calibration of neutron measuring devices. In this work, the neutron calibration fields were investigated in terms of neutron energy spectra and dose equivalent rates using Monte Carlo simulations, an in-house developed neutron spectrometer and commercial survey meters. The characterized neutron fields can generate neutron dose equivalent rates ranging from 156 μSv/h to 3.5 mSv/h with nearly 100% of dose contributed by neutrons of energies larger than 0.01 MeV. The gamma contamination was less than 4.2-7.5% depending on the irradiation configuration. It is possible to use the described neutron fields for calibration test and routine quality assurance of neutron dose rate meters and passive dosemeters commonly used in radiation protection dosimetry.

Assessment of the global fallout of plutonium isotopes and americium-241 in the soil of the central region of Saudi Arabia.

PubMed

Shabana, E I; Al-Shammari, H L

2001-01-01

A radiochemical technique for determination of plutonium isotopes and 241Am in soil samples is tested against IAEA-standard reference materials to determine its accuracy and precision for reliable results. The technique is then used in the investigation of topsoil samples, collected from the natural environment of the central region of Saudi Arabia, to assess the effect of fallout accumulation of these radionuclides in the region. Plutonium and americium were sequentially separated from all other components of the sample by anion-exchange chromatography and co-precipitated with Nd3+ as fluorides. The precipitates were mounted on membrane filters and measured using a high-resolution alpha-spectrometer. The results of the analysis of the reference materials showed satisfactory sensitivity and precision of the technique. The results of the analyzed soil samples show activity levels ranging from < LLD to 0.089 and from

Electrochemical reduction of (U-40Pu-5Np)O 2 in molten LiCl electrolyte

NASA Astrophysics Data System (ADS)

Iizuka, Masatoshi; Sakamura, Yoshiharu; Inoue, Tadashi

2006-12-01

The electrochemical reduction of neptunium-containing MOX ((U-40Pu-5Np)O 2) was performed in molten lithium chloride melt at 923 K to investigate fundamental behavior of the transuranium elements and applicability of the method to reduction process for these materials. The Np-MOX was electrochemically reduced at the potential lower than -0.6 V vs. Bi-35 mol% Li reference electrode. The reduced metal grains in the surface region of the sample cohered with each other and made the layer of relatively high density, although it did not prevent the reduction of the sample toward the center. Complete reduction of the Np-MOX was shown by the weight change measurement through the electrochemical reduction and also by SEM-EDX observation. The chemical composition of the reduction products was homogeneous and agreed to that of the initial Np-MOX, which indicates that the reduction was completed and not selective among the actinides. The concentrations of the actinide elements, especially plutonium and americium in the electrolyte, increased with the progress of the tests, although their absolute values were very small. It is quite likely that plutonium and americium dissolve into the melt in the same manner as the lanthanide elements in the lithium reduction process.

Device and method for accurately measuring concentrations of airborne transuranic isotopes

DOEpatents

McIsaac, Charles V.; Killian, E. Wayne; Grafwallner, Ervin G.; Kynaston, Ronnie L.; Johnson, Larry O.; Randolph, Peter D.

1996-01-01

An alpha continuous air monitor (CAM) with two silicon alpha detectors and three sample collection filters is described. This alpha CAM design provides continuous sampling and also measures the cumulative transuranic (TRU), i.e., plutonium and americium, activity on the filter, and thus provides a more accurate measurement of airborne TRU concentrations than can be accomplished using a single fixed sample collection filter and a single silicon alpha detector.

BAG PASSOUT SEALER FOR WATER-SHIELDED CAVE FACILITY (Engineering Materials)

DOE Office of Scientific and Technical Information (OSTI.GOV)

None

1963-10-31

The water-shielded cave facility is used in processing irradiated slugs for recovery of americium, curium, berkelium, californium, einsteinium, and fermium. The remotely operated, plastic-bag passout sealer is used in removing isotopic fractions for storage in the rear or for removing radioactive waste for placement in the waste storage containers. The unit is accessible by both the primary inclosure master-slaves and the service area master-slaves. (F.L.S.)

Processing plutonium-contaminated soil on Johnston Atoll

DOE Office of Scientific and Technical Information (OSTI.GOV)

Moroney, K.; Moroney, J. III; Turney, J.

1994-07-01

This article describes a cleanup project to process plutonium- and americium-contaminated soil on Johnston Atoll for volume reduction. Thermo Analytical`s (TMA`s) segmented gate system (SGS) for this remedial operation has been in successful on-site operation since 1992. Topics covered include the basis for development, a description of the Johnston Atoll; the significance of results; the benefits of the technology; applicability to other radiologically contaminated sites. 7 figs., 1 tab.

Defense Horizons. Number 38, January 2004. Dirty Bombs: The Threat Revisited

DTIC Science & Technology

2004-01-01

plutonium-238 (238Pu), americium - 241 (241Am), and cali- fornium-252 (252Cf). Types of Damage Deterministic Injuries. Radiation is said to cause...megasources” such as Russian radioisotope thermal generators ( RTGs ) and Gamma-Kolos seed irradiators. By far the most likely route for terrorist...facility or a business or residential district, not just open space . More efficient RDDs relying on other means to disseminate the same amount of

Research in radiobiology. Annual report of work in progress in the internal irradiation program

DOE Office of Scientific and Technical Information (OSTI.GOV)

Not Available

1979-03-31

The toxicity, retention, biological effects, distribution, decorporation and measuring techniques of radionuclides are discussed. Calculations of trabecular bone formation rates from tetracycline labeling is included. The characteristics of trabecular bone in the Rhesus monkey are discussed. Studies on the early retention and distribution of radium 224 in beagles are included. Studies on the decorporation of plutonium and americium in dogs by DTPA and salicylic acid are presented.

Device and method for accurately measuring concentrations of airborne transuranic isotopes

DOEpatents

McIsaac, C.V.; Killian, E.W.; Grafwallner, E.G.; Kynaston, R.L.; Johnson, L.O.; Randolph, P.D.

1996-09-03

An alpha continuous air monitor (CAM) with two silicon alpha detectors and three sample collection filters is described. This alpha CAM design provides continuous sampling and also measures the cumulative transuranic (TRU), i.e., plutonium and americium, activity on the filter, and thus provides a more accurate measurement of airborne TRU concentrations than can be accomplished using a single fixed sample collection filter and a single silicon alpha detector. 7 figs.

Features of the Thermodynamics of Trivalent Lanthanide/Actinide Distribution Reactions by Tri-n-Octylphosphine Oxide and Bis(2-EthylHexyl) Phosphoric Acid

DOE Office of Scientific and Technical Information (OSTI.GOV)

Travis S. Grimes; Peter R. Zalupski

2014-11-01

A new methodology has been developed to study the thermochemical features of the biphasic transfer reactions of trisnitrato complexes of lanthanides and americium by a mono-functional solvating ligand (tri-n-octyl phosphine oxide - TOPO). Stability constants for successive nitrato complexes (M(NO3)x3-x (aq) where M is Eu3+, Am3+ or Cm3+) were determined to assist in the calculation of the extraction constant, Kex, for the metal ions under study. Enthalpies of extraction (?Hextr) for the lanthanide series (excluding Pm3+) and Am3+ by TOPO have been measured using isothermal titration calorimetry. The observed ?Hextr were found to be constant at ~29 kJ mol-1across themore » series from La3+-Er3+, with a slight decrease observed from Tm3+-Lu3+. These heats were found to be consistent with enthalpies determined using van ’t Hoff analysis of temperature dependent extraction studies. A complete set of thermodynamic parameters (?G, ?H, ?S) was calculated for Eu(NO3)3, Am(NO3)3 and Cm(NO3)3 extraction by TOPO and Am3+ and Cm3+ extraction by bis(2-ethylhexyl) phosphoric acid (HDEHP). A discussion comparing the energetics of these systems is offered. The measured biphasic extraction heats for the transplutonium elements, ?Hextr, presented in these studies are the first ever direct measurements offered using two-phase calorimetric techniques.« less

Chemistry of berkelium: A review

NASA Astrophysics Data System (ADS)

Hobart, D. E.; Peterson, J. R.

Element 97 was first produced in December 1949, by the bombardment of americium-241 with accelerated alpha particles. This new element was named berkelium (Bk) after Berkeley, California, the city of its discovery. In the 36 years since the discovery of Bk, a substantial amount of knowledge concerning the physicochemical properties of this relatively scarce transplutonium element was acquired. All of the Bk isotopes of mass numbers 240 and 242 through 251 are presently known, but only berkelium-249 is available in sufficient quantities for bulk chemical studies. About 0.7 gram of this isotope was isolated at the HFIR/TRU Complex in Oak Ridge, Tennessee in the last 18 years. Over the same time period, the scale of experimental work using berkelium-249 has increased from the tracer level to bulk studies at the microgram level to solution and solid state investigations with milligram quantities. Extended knowledge of the physicochemical behavior of berkelium is important in its own right, because Bk is the first member of the second half of the actinide series. In addition, such information should enable more accurate extrapolations to the predicted behavior of heavier elements for which experimental studies are severely limited by lack of material and/or by intense radioactivity.

Americium, plutonium and uranium contamination and speciation in well waters, streams and atomic lakes in the Sarzhal region of the Semipalatinsk Nuclear Test Site, Kazakhstan.

PubMed

León Vintró, L; Mitchell, P I; Omarova, A; Burkitbayev, M; Jiménez Nápoles, H; Priest, N D

2009-04-01

New data are reported on the concentrations, isotopic composition and speciation of americium, plutonium and uranium in surface and ground waters in the Sarzhal region of the Semipalatinsk Test Site, and an adjacent area including the settlement of Sarzhal. The data relate to filtered water and suspended particulate from (a) streams originating in the Degelen Mountains, (b) the Tel'kem 1 and Tel'kem 2 atomic craters, and (c) wells on farms located within the study area and at Sarzhal. The measurements show that (241)Am, (239,240)Pu and (238)U concentrations in well waters within the study area are in the range 0.04-87mBq dm(-3), 0.7-99mBq dm(-3), and 74-213mBq dm(-3), respectively, and for (241)Am and (239,240)Pu are elevated above the levels expected solely on the basis of global fallout. Concentrations in streams sourced in the Degelen Mountains are similar, while concentrations in the two water-filled atomic craters are somewhat higher. Suspended particulate concentrations in well waters vary considerably, though median values are very low, at 0.01mBq dm(-3), 0.08mBq dm(-3) and 0.32mBq dm(-3) for (241)Am, (239,240)Pu and (238)U, respectively. The (235)U/(238)U isotopic ratio in almost all well and stream waters is slightly elevated above the 'best estimate' value for natural uranium worldwide, suggesting that some of the uranium in these waters is of test-site provenance. Redox analysis shows that on average most of the plutonium present in the microfiltered fraction of these waters is in a chemically reduced form (mean 69%; 95% confidence interval 53-85%). In the case of the atomic craters, the proportion is even higher. As expected, all of the americium present appears to be in a reduced form. Calculations suggest that annual committed effective doses to individual adults arising from the daily ingestion of these well waters are in the range 11-42microSv (mean 21microSv). Presently, the ground water feeding these wells would not appear to be contaminated with radioactivity from past underground testing in the Degelen Mountains or from the Tel'kem explosions.

Americium-241 Decorporation Model

DTIC Science & Technology

2014-10-01

doses compared Radiation Dose Convert mass to activity if needed Calculate critical organ doses/ effective whole body dose (Christy and Eckerman...compartments over time with and without treatment, excretion rates, and radiation doses to critical organs. Calculations from the model may be used to...268 x E + 2 newton-meter (N/m) pound-force/foot2 4.788 026 x E – 2 kilo pascal (kPa) pound-force/inch2 (psi) 6.894 757 kilo pascal (kPa) pound- mass

Determination of Pu and 241Am in soils by instrumental methods

NASA Astrophysics Data System (ADS)

Yaroshevich, O. J.; Zhuk, I. V.; Lomonosova, E. M.; Svetlakova, N. N.; Mironov, V. P.; Kudryashov, V. P.; Bushuev, A. V.

1995-06-01

A method based on the detection of x- and low energy γ-radiation for determining the activity of plutonium and americium-241 in soils and sediments is described. The results of x- and γ-radiation spectral measurements are presented. Possible ways to increase the sensitivity of the method are discussed. The results of measurements of α-particle activity distributions with solid state nuclear track detectors for depth profiling of different types of soils are also presented.

Semiconductor quantum dot scintillation under gamma-ray irradiation.

PubMed

Létant, S E; Wang, T-F

2006-12-01

We recently demonstrated the ability of semiconductor quantum dots to convert alpha radiation into visible photons. In this letter, we report on the scintillation of quantum dots under gamma irradiation and compare the energy resolution of the 59 keV line of americium-241 obtained with our quantum dot-glass nanocomposite to that of a standard sodium iodide scintillator. A factor 2 improvement is demonstrated experimentally and interpreted theoretically using a combination of energy-loss and photon-transport models.

Separation of Californium from other Actinides

DOEpatents

Mailen, J C; Ferris, L M

1973-09-25

A method is provided for separating californium from a fused fluoride composition containing californium and at least one element selected from the group consisting of plutonium, americium, curium, uranium, thorium, and protactinium which comprises contacting said fluoride composition with a liquid bismuth phase containing sufficient lithium or thorium to effect transfer of said actinides to the bismuth phase and then contacting the liquid bismuth phase with molten LiCl to effect selective transfer of californium to the chloride phase.

Accomplishing Equilibrium in ALSEP: Demonstrations of Modified Process Chemistry on 3-D Printed Enhanced Annular Centrifugal Contactors

DOE PAGES

Brown, M. Alex; Wardle, Kent E.; Lumetta, Gregg; ...

2016-12-01

Here, the major components of the modified ALSEP process have been demonstrated on a modified 2-cm annular centrifugal contactor with an enhanced mixing zone using stable fission products and radiotracers. The results show that by decreasing the pH of the minor actinide stripping solution, using HEDTA instead of DTPA, and increasing contact time, the process is very effective in separating americium from the lanthanides and the fission products.

Environmental Impact Statement for BOMARC Missile Site, McGuire AFB, New Jersey. Volume 1, Sections 1 through 8

DTIC Science & Technology

1992-05-22

laboratory analysis and in-situ survey techniques . It is estimated that the radiological surveys would generate four 55-gallon drums of potentially...the filters would be analyzed daily in the field for alpha activity. If air filter analysis indicates resuspension of plutonium and/or americium...successional change would eventually result in the old field vegetative zone developing into an Oak-Pine community or an oak-hickory climax community

Covalency in Americium(III) Hexachloride

DOE PAGES

Cross, Justin Neil; Su, Jing; Batista, Enrigue R.; ...

2017-06-14

Developing a better understanding of covalency (or orbital mixing) is of fundamental importance. Covalency occupies a central role in directing chemical and physical properties for almost any given compound or material. Hence, the concept of covalency has potential to generate broad and substantial scientific advances, ranging from biological applications to condensed matter physics. Given the importance orbital mixing combined with the difficultly in measuring covalency, estimating or inferring covalency often leads to fiery debate. Consider the 60-year controversy sparked by SEABORG and COWORKERS (1954) when it was proposed that covalency from 5f-orbitals contributed to the unique behavior of americium inmore » chloride matrixes. Herein, we describe the use of ligand K-edge X-ray absorption spectroscopy (XAS) and electronic structure calculations to quantify the extent of covalent bonding in – arguably – one of the most difficult systems to study, the Am–Cl interaction within AmCl 6 3-. We observed both 5fand 6d-orbital mixing with the Cl-3p orbitals; however, contributions from the 6d-orbitals were more substantial. Comparisons with the isoelectronic EuCl 6 3- indicated similar bonding for the Am III 6d- and Eu III 5d-orbitals. Meanwhile, the results confirmed SEABORG’S 1954 hypothesis that Am III 5f-orbital covalency was more substantial than 4forbital mixing for Eu III.« less

Factors affecting the availability of americium-241 to the rice plant

DOE Office of Scientific and Technical Information (OSTI.GOV)

Adriano, D.C.

1979-11-01

Since there has been no published transuranic uptake data on the rice plant (Oryza sativa L.), greenhouse experiments were conducted to determine the effects of some factors on the uptake of /sup 241/Am by this crop. Results indicate that chelated /sup 241/Am (in the form of americium-241-diethylenetriaminepentaacetic acid) applied to the flood water was markedly taken up by the rice plant, compared to the nonchelated form. However, most of the accumulation of /sup 241/Am occurred in the vegetative parts and only trace amounts, if any, were translocated to the grain. Soil application of /sup 241/Am resulted in much lower uptake.more » Soil amendment with either diethylenetriaminepentaacetic acid (DTPA) or organic matter did not produce a discernible uptake pattern. A synthesis of published data on plant uptake of /sup 241/Am indicates that the concentration ratio (CR, a measure of availability of /sup 241/Am to the plants) values for /sup 241/Am for agricultural crops ranged from 10-/sup 6/ to 10/sup 1/ (from lowest to highest availability). Some factors that appear to influence /sup 241/Am uptake are as follows: plant parts (grain usually having lower CR), chelating agents (DTPA usually increasing the CR), organic matter (inconsistent effects although generally decreasing the CR), and lime (usually decreasing the CR).« less

Americium(III) capture using phosphonic acid-functionalized silicas with different mesoporous morphologies: adsorption behavior study and mechanism investigation by EXAFS/XPS.

PubMed

Zhang, Wen; He, Xihong; Ye, Gang; Yi, Rong; Chen, Jing

2014-06-17

Efficient capture of highly toxic radionuclides with long half-lives such as Americium-241 is crucial to prevent radionuclides from diffusing into the biosphere. To reach this purpose, three different types of mesoporous silicas functionalized with phosphonic acid ligands (SBA-POH, MCM-POH, and BPMO-POH) were synthesized via a facile procedure. The structure, surface chemistry, and micromorphology of the materials were fully characterized by (31)P/(13)C/(29)Si MAS NMR, XPS, and XRD analysis. Efficient adsorption of Am(III) was realized with a fast rate to reach equilibrium (within 10 min). Influences including structural parameters and functionalization degree on the adsorption behavior were investigated. Slope analysis of the equilibrium data suggested that the coordination with Am(III) involved the exchange of three protons. Moreover, extended X-ray absorption fine structure (EXAFS) analysis, in combination with XPS survey, was employed for an in-depth probe into the binding mechanism by using Eu(III) as a simulant due to its similar coordination behavior and benign property. The results showed three phosphonic acid ligands were coordinated to Eu(III) in bidentate fashion, and Eu(P(O)O)3(H2O) species were formed with the Eu-O coordination number of 7. These phosphonic acid-functionalized mesoporous silicas should be promising for the treatment of Am-containing radioactive liquid waste.

The coprecipitation of Pu and other radionuclides with CaCO[sub 3

DOE Office of Scientific and Technical Information (OSTI.GOV)

Meece, D.E.; Benninger, L.K.

1993-04-01

The record of fallout plutonium concentrations in annual bands of corals is strikingly similar to the record of atmospheric deposition of [sup 90]Sr. This similarity implies that corals may incorporate Pu from seawater with a constant partition coefficient (constant discrimination). To investigate physicochemical aspects of Pu incorporation, the following have been coprecipitated with CaCO[sub 3] (calcite and aragonite): oxidized and reduced Pu; americium, thorium, and uranium as analogs to Pu oxidation states (III, IV, VI), respectively; and [sup 210]Pb as a particle-reactive nuclide which may be incorporated by corals with constant discrimination. Americium, thorium, and lead adsorb onto both calcitemore » and aragonite, with more than 99% of the recovered activity found associated with the solids. Uranium exhibits a behavior consistent with lattice substitution. Partition coefficients for U in aragonite range from 1.8 to 9.8 and vary inversely with pH and/or rate of precipitation. The partition coefficient for U in calcite is less than 0.2 and may be as low as 0.046. Reduced Pu sorbs with 3 to 4% remaining in solution. Oxidized Pu may both sorb and coprecipitate. The coral record for Pb and U results primarily from biological, rather than physicochemical, effects; it is likely that the PU coral record also reflects biological discrimination. 50 refs., 4 figs., 5 tabs.« less

The United States Transuranium and Uranium Registries. Revision 1, [Annual] report, October 1, 1990--April 1992

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kathren, R.L.

1992-09-01

This paper describes the history, organization, activities and recent scientific accomplishments of the United States Transuranium and Uranium Registries. Through voluntary donations of tissue obtained at autopsies, the Registries carry out studies of the concentration, distribution and biokinetics of plutonium in occupationally exposed persons. Findings from tissue analyses from more than 200 autopsies include the following: a greater proportion of the americium intake, as compared with plutonium, was found in the skeleton; the half-time of americium in liver is significantly shorter than that of plutonium; the concentration of actinide in the skeleton is inversely proportional to the calcium and ashmore » content of the bone; only a small percentage of the total skeletal deposition of plutonium is found in the marrow, implying a smaller risk from irradiation of the marrow relative to the bone surfaces; estimates of plutonium body burden made from urinalysis typically exceed those made from autopsy data; pathologists were unable to discriminate between a group of uranium workers and persons without known occupational exposure on the basis of evaluation of microscopic kidney slides; the skeleton is an important long term depot for uranium, and that the fractional uptake by both skeleton and kidney may be greater than indicated by current models. These and other findings and current studies are discussed in depth.« less

In Vitro Dissolution Tests of Plutonium and Americium Containing Contamination Originating From ZPPR Fuel Plates

DOE Office of Scientific and Technical Information (OSTI.GOV)

William F. Bauer; Brian K. Schuetz; Gary M. Huestis

2012-09-01

Assessing the extent of internal dose is of concern whenever workers are exposed to airborne radionuclides or other contaminants. Internal dose determinations depend upon a reasonable estimate of the expected biological half-life of the contaminants in the respiratory tract. One issue with refractory elements is determining the dissolution rate of the element. Actinides such as plutonium (Pu) and Americium (Am) tend to be very refractory and can have biological half-lives of tens of years. In the event of an exposure, the dissolution rates of the radionuclides of interest needs to be assessed in order to assign the proper internal dosemore » estimates. During the November 2011 incident at the Idaho National Laboratory (INL) involving a ZPPR fuel plate, air filters in a constant air monitor (CAM) and a giraffe filter apparatus captured airborne particulate matter. These filters were used in dissolution rate experiments to determine the apparent dissolution half-life of Pu and Am in simulated biological fluids. This report describes these experiments and the results. The dissolution rates were found to follow a three term exponential decay equation. Differences were noted depending upon the nature of the biological fluid simulant. Overall, greater than 95% of the Pu and 93% of the Am were in a very slow dissolving component with dissolution half-lives of over 10 years.« less

Quantum size effects on the (0001) surface of double hexagonal close packed americium

NASA Astrophysics Data System (ADS)

Gao, D.; Ray, A. K.

2007-01-01

Electronic structures of double hexagonal close-packed americium and the (0001) surface have been studied via full-potential all-electron density-functional calculations with a mixed APW+lo/LAPW basis. The electronic and geometric properties of bulk dhcp Am as well as quantum size effects in the surface energies and the work functions of the dhcp Am (0001) ultra thin films up to seven layers have been examined at nonmagnetic, ferromagnetic, and antiferromagnetic configurations with and without spin orbit coupling. The anti-ferromagnetic state including spin-orbit coupling is found to be the ground state of dhcp Am with the 5f electrons primarily localized. Our results show that both magnetic configurations and spin-orbit coupling play important roles in determining the equilibrium lattice constant, the bulk modulus as well as the localized feature of 5f electrons for dhcp Am. Our calculated equilibrium lattice constant and bulk modulus at the ground state are in good agreement with the experimental values respectively. The work function of dhcp Am (0001) 7-layer surface at the ground state is predicted to be 2.90 eV. The surface energy for dhcp Am (0001) semi-infinite surface energy at the ground state is predicted to be 0.84 J/m2. Quantum size effects are found to be more pronounced in work functions than in surface energies.

METHOD OF ALLOYING REACTIVE METALS WITH ALUMINUM OR BERYLLIUM

DOEpatents

Runnalls, O.J.C.

1957-10-15

A halide of one or more of the reactive metals, neptunium, cerium and americium, is mixed with aluminum or beryllium. The mass is heated at 700 to 1200 deg C, while maintaining a substantial vacuum of above 10/sup -3/ mm of mercury or better, until the halide of the reactive metal is reduced and the metal itself alloys with the reducing metal. The reaction proceeds efficiently due to the volatilization of the halides of the reducing metal, aluminum or beryllium.

Removal of radioactive and other hazardous material from fluid waste

DOEpatents

Tranter, Troy J [Idaho Falls, ID; Knecht, Dieter A [Idaho Falls, ID; Todd, Terry A [Aberdeen, ID; Burchfield, Larry A [W. Richland, WA; Anshits, Alexander G [Krasnoyarsk, RU; Vereshchagina, Tatiana [Krasnoyarsk, RU; Tretyakov, Alexander A [Zheleznogorsk, RU; Aloy, Albert S [St. Petersburg, RU; Sapozhnikova, Natalia V [St. Petersburg, RU

2006-10-03

Hollow glass microspheres obtained from fly ash (cenospheres) are impregnated with extractants/ion-exchangers and used to remove hazardous material from fluid waste. In a preferred embodiment the microsphere material is loaded with ammonium molybdophosphonate (AMP) and used to remove radioactive ions, such as cesium-137, from acidic liquid wastes. In another preferred embodiment, the microsphere material is loaded with octyl(phenyl)-N-N-diisobutyl-carbamoylmethylphosphine oxide (CMPO) and used to remove americium and plutonium from acidic liquid wastes.

Reanalysis of Plutonium and Americium-241 in the Tank 19F Closure Grab and Core Samples

DOE Office of Scientific and Technical Information (OSTI.GOV)

Swingle, R.F.

2003-02-11

Tank 19F is scheduled to be closed by March 2004. To close this tank, a characterization of the waste remaining in the tank was required to confirm the inventory of various species for input into groundwater transport models. This characterization has been developed by a combination of process knowledge, visual observation and sample analysis. The characterization samples were obtained by High Level Waste Division (HLWD) personnel and characterized by SRTC personnel.

Measurement system for alpha emitters in solution

NASA Astrophysics Data System (ADS)

Robert, A.; Sella, C.; Heindl, R.

1984-08-01

The measurement of alpha emitter concentrations in solution corresponds to a need felt in particular by laboratories working on actinides and in the spent fuel reprocessing industry. The instrument present here allows this measurement continuously by the use of a new scintillator that is insensitive to corrosive liquids. The extreme thinness of the scintillator guarantees good detection selectivity of alpha particles in the presence of beta and gamma emissions. Examples of uranium-233, plutonium-239 and americium-241 concentration measurements are presented.

Development and Use of an X-ray Induced Fluorescence System Designed to Measure Regional Myocardial Perfusion

DTIC Science & Technology

1989-08-01

1969] to measure iodine concentration in the thyroid gland. An americium - 241 source was used to induce the fluorescence of iodine which had...Report No. TR 91-010 October 1991 Supported by: L.R. Hettche, Director Space and Naval Warfare Systems Command Applied Research Laboratory Approved...Laboratory P.O. Box 30 TR# 91-010 State College, PA 16804 ". SPONSOIUNG; MONITONG AGENCY NAM(S) ANO ADORESS(ES) Ia. SiINSO -4 /IOWI mI Space and Naval

Natural Transmutation of Actinides via the Fission Reaction in the Closed Thorium-Uranium-Plutonium Fuel Cycle

NASA Astrophysics Data System (ADS)

Marshalkin, V. Ye.; Povyshev, V. M.

2017-12-01

It is shown for a closed thorium-uranium-plutonium fuel cycle that, upon processing of one metric ton of irradiated fuel after each four-year campaign, the radioactive wastes contain 54 kg of fission products, 0.8 kg of thorium, 0.10 kg of uranium isotopes, 0.005 kg of plutonium isotopes, 0.002 kg of neptunium, and "trace" amounts of americium and curium isotopes. This qualitatively simplifies the handling of high-level wastes in nuclear power engineering.

Brief overview of the long-lived radionuclide separation processes developed in france in connection with the spin program

NASA Astrophysics Data System (ADS)

Madic, Charles; Bourges, Jacques; Dozol, Jean-François

1995-09-01

To reduce the long-term potential hazards associated with the management of nuclear wastes generated by nuclear fuel reprocessing, one alternative is the transmutation of long-lived radionuclides into short-lived radionuclides by nuclear means (P & T strategy). In this context, according to the law passed by the French Parliament on 30 December 1991, the CEA launched the SPIN program for the design of long-lived radionuclide separation and nuclear incineration processes. The research in progress to define separation processes focused mainly on the minor actinides (neptunium, americium and curium) and some fission products, like cesium and technetium. To separate these long-lived radionuclides, two strategies were developed. The first involves research on new operating conditions for improving the PUREX fuel reprocessing technology. This approach concerns the elements neptunium and technetium (iodine and zirconium can also be considered). The second strategy involves the design of new processes; DIAMEX for the co-extraction of minor actinides from the high-level liquid waste leaving the PUREX process, An(III)/Ln(III) separation using tripyridyltriazine derivatives or picolinamide extracting agents; SESAME for the selective separation of americium after its oxidation to Am(IV) or Am(VI) in the presence of a heteropolytungstate ligand, and Cs extraction using a new class of extracting agents, calixarenes, which exhibit exceptional Cs separation properties, especially in the presence of sodium ion. This lecture focuses on the latest achievements in these research areas.

Production and investigation of thin films of metal actinides (Pu, Am, Cm, Bk, Cf)

NASA Astrophysics Data System (ADS)

Radchenko, V. M.; Ryabinin, M. A.; Stupin, V. A.

2010-03-01

Under limited availability of transplutonium metals some special techniques and methods of their production have been developed that combine the process of metal reduction from a chemical compound and preparation of a sample for examination. In this situation the evaporation and condensation of metal onto a substrate becomes the only possible technology. Thin film samples of metallic 244Cm, 248Cm and 249Bk were produced by thermal reduction of oxides with thorium followed by deposition of the metals in the form of thin layers on tantalum substrates. For the production of 249Cf metal in the form of a thin layer the method of thermal reduction of oxide with lanthanum was used. 238Pu and 239Pu samples in the form of films were prepared by direct high temperature evaporation and condensation of the metal onto a substrate. For the production of 241Am films a gram sample of plutonium-241 metal was used containing about 18 % of americium at the time of production. Thermal decomposition of Pt5Am intermetallics in vacuum was used to produce americium metal with about 80% yield. Resistivity of the metallic 249Cf film samples was found to decrease exponentially with increasing temperature. The 249Cf metal demonstrated a tendency to form preferably a DHCP structure with the sample mass increasing. An effect of high specific activity on the crystal structure of 238Pu nuclide thin layers was studied either.

Waste Isolation Pilot Plant Salt Decontamination Testing

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rick Demmer; Stephen Reese

2014-09-01

On February 14, 2014, americium and plutonium contamination was released in the Waste Isolation Pilot Plant (WIPP) salt caverns. At the request of WIPP’s operations contractor, Idaho National Laboratory (INL) personnel developed several methods of decontaminating WIPP salt, using surrogate contaminants and also americium (241Am). The effectiveness of the methods is evaluated qualitatively, and to the extent possible, quantitatively. One of the requirements of this effort was delivering initial results and recommendations within a few weeks. That requirement, in combination with the limited scope of the project, made in-depth analysis impractical in some instances. Of the methods tested (dry brushing,more » vacuum cleaning, water washing, strippable coatings, and mechanical grinding), the most practical seems to be water washing. Effectiveness is very high, and it is very easy and rapid to deploy. The amount of wastewater produced (2 L/m2) would be substantial and may not be easy to manage, but the method is the clear winner from a usability perspective. Removable surface contamination levels (smear results) from the strippable coating and water washing coupons found no residual removable contamination. Thus, whatever is left is likely adhered to (or trapped within) the salt. The other option that shows promise is the use of a fixative barrier. Bartlett Nuclear, Inc.’s Polymeric Barrier System (PBS) proved the most durable of the coatings tested. The coatings were not tested for contaminant entrapment, only for coating integrity and durability.« less

Colloid-facilitated radionuclide transport: a regulatory perspective

NASA Astrophysics Data System (ADS)

Dam, W. L.; Pickett, D. A.; Codell, R. B.; Nicholson, T. J.

2001-12-01

What hydrogeologic-geochemical-microbial conditions and processes affect migration of radionuclides sorbed onto microparticles or native colloid-sized radionuclide particles? The U.S. Nuclear Regulatory Commission (NRC) is responsible for protecting public health, safety, and the environment at numerous nuclear facilities including a potential high-level nuclear waste disposal site. To fulfill these obligations, NRC needs to understand the mechanisms controlling radionuclide release and transport and their importance to performance. The current focus of NRC staff reviews and technical interactions dealing with colloid-facilitated transport relates to the potential nuclear-waste repository at Yucca Mountain, Nevada. NRC staff performed bounding calculations to quantify radionuclide releases available for ground-water transport to potential receptors from a Yucca Mountain repository. Preliminary analyses suggest insignificant doses of plutonium and americium colloids could be derived from spent nuclear fuel. Using surface complexation models, NRC staff found that colloids can potentially lower actinide retardation factors by up to several orders of magnitude. Performance assessment calculations, in which colloidal transport of plutonium and americium was simulated by assuming no sorption or matrix diffusion, indicated no effect of colloids on human dose within the 10,000 year compliance period due largely to long waste-package lifetimes. NRC staff have identified information gaps and developed technical agreements with the U.S. Department of Energy (DOE) to ensure sufficient information will be presented in any potential future Yucca Mountain license application. DOE has agreed to identify which radionuclides could be transported via colloids, incorporate uncertainties in colloid formation, release and transport parameters, and conceptual models, and address the applicability of field data using synthetic microspheres as colloid analogs. NRC is currently investigating approaches to colloid modeling in order to help evaluate DOE's approach. One alternative approach uses DOE laboratory data to invoke kinetic controls on reversible radionuclide attachment to colloids. A kinetic approach in which desorption from colloids is slow may help assess whether DOE's instantaneous equilibrium approach for reversible attachment, as well as their application of irreversible attachment to only a small portion of the radionuclide inventory, are reasonable and conservative. An approach to examine microbial processes would also contribute to considerations of leaching of radionuclides and colloid formation. Reducing uncertainties in colloid transport processes should help in better understanding their importance to repository performance. This work is an independent product and does not necessarily reflect the views or regulatory position of the NRC. CNWRA participation was funded under contract No. NRC-02-97-009.

Method for the recovery of actinide elements from nuclear reactor waste

DOEpatents

Horwitz, E. Philip; Delphin, Walter H.; Mason, George W.

1979-01-01

A process for partitioning and recovering actinide values from acidic waste solutions resulting from reprocessing of irradiated nuclear fuels by adding hydroxylammonium nitrate and hydrazine to the waste solution to adjust the valence of the neptunium and plutonium values in the solution to the +4 oxidation state, thus forming a feed solution and contacting the feed solution with an extractant of dihexoxyethyl phosphoric acid in an organic diluent whereby the actinide values, most of the rare earth values and some fission product values are taken up by the extractant. Separation is achieved by contacting the loaded extractant with two aqueous strip solutions, a nitric acid solution to selectively strip the americium, curium and rare earth values and an oxalate solution of tetramethylammonium hydrogen oxalate and oxalic acid or trimethylammonium hydrogen oxalate to selectively strip the neptunium, plutonium and fission product values. Uranium values remain in the extractant and may be recovered with a phosphoric acid strip. The neptunium and plutonium values are recovered from the oxalate by adding sufficient nitric acid to destroy the complexing ability of the oxalate, forming a second feed, and contacting the second feed with a second extractant of tricaprylmethylammonium nitrate in an inert diluent whereby the neptunium and plutonium values are selectively extracted. The values are recovered from the extractant with formic acid.

Removal of Cesium From Acidic Radioactive Tank Waste Using IONSIV IE-911 (CST)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mann, Nicholas Robert; Todd, Terry Allen

2004-10-01

IONSIV IE-911, or the engineered form of crystalline silicotitanate (CST), manufactured by UOP Molecular Sieves, has been evaluated for the removal of cesium from Idaho National Engineering and Environmental Laboratory (INEEL) acidic radioactive tank waste. A series of batch contacts and column tests were performed by using three separate batches of CST. Batch contacts were performed to evaluate the concentration effects of nitric acid, sodium, and potassium ions on cesium sorption. Additional batch tests were performed to determine if americium, mercury, and plutonium would sorb onto IONSIV IE-911. An equilibrium isotherm was generated by using a concentrated tank waste simulant.more » Column tests using a 1.5 cm 3 column and flow rates of 3, 5, 10, 20, and 30 bed volumes (BV)/hr were performed to elucidate dynamic cesium sorption capacities and sorption kinetics. Additional experiments investigated the effect of CST batch and pretreatment on cesium sorption. The thermal stability of IONSIV IE-911 was evaluated by performing thermal gravimetric analysis/differential thermal analysis. Overall, IONSIV IE-911 was shown to be effective for cesium sorption from complex, highly acidic solutions; however, sorbent stability in these solutions may have a deleterious effect on cesium sorption.« less

Development of an integrated transuranic waste management system for a large research facility: NUCEF

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mineo, Hideaki; Matsumura, Tatsuro; Takeshita, Isao

1997-03-01

The Nuclear Fuel Cycle Safety Engineering Research Facility (NUCEF) is a large complex of research facilities where transuranic (TRU) elements are used. Liquid and solid waste containing TRU elements is generated mainly in the treatment of fuel for critical experiments and in the research of reprocessing and TRU waste management in hot cells and glove boxes. The rational management of TRU wastes is a very important issue not only for NUCEF but also for Japan. An integrated TRU waste management system is being developed with NUCEF as the test bed. The basic policy for establishing the system is to classifymore » wastes by TRU concentration, to reduce waste volume, and to maximize reuse of TRU elements. The principal approach of the development program is to apply the outcomes of the research carried out in NUCEF. Key technologies are TRU measurement for classification of solid wastes and TRU separation and volume reduction for organic and aqueous wastes. Some technologies required for treating the wastes specific to the research activities in NUCEF need further development. Specifically, the separation and stabilization technologies for americium recovery from concentrated aqueous waste, which is generated in dissolution of mixed oxide when preparing fuel for critical experiments, needs further research.« less

Diethylene-triamine-penta-acetate administration protocol for radiological emergency medicine in nuclear fuel reprocessing plants.

PubMed

Jin, Yutaka

2008-01-01

Inhalation therapy of diethylene-triamine-penta-acetate (DTPA) should be initiated immediately to workers who have significant incorporation of plutonium, americium or curium in the nuclear fuel reprocessing plant. A newly designed electric mesh nebulizer is a small battery-operated passive vibrating mesh device, in which vibrations in an ultrasonic horn are used to force drug solution through a mesh of micron-sized holes. This nebulizer enables DTPA administration at an early stage in the event of a radiation emergency from contamination from the above radioactive metals.

Radionuclide concentrations in honey bees from Area G at TA-54 during 1997. Progress report

DOE Office of Scientific and Technical Information (OSTI.GOV)

Haarmann, T.K.; Fresquez, P.R.

Honey bees were collected from two colonies located at Los Alamos National Laboratory`s Area G, Technical Area 54, and from one control (background) colony located near Jamez Springs, NM. Samples were analyzed for the following: cesium ({sup 137}Cs), americium ({sup 241}Am), plutonium ({sup 238}Pu and {sup 239,240}Pu), tritium ({sup 3}H), total uranium, and gross gamma activity. Area G sample results from both colonies were higher than the upper (95%) level background concentration for {sup 238}Pu and {sup 3}H.

METHOD OF MAKING ALLOYS OF BERYLLIUM WITH PLUTONIUM AND THE LIKE

DOEpatents

Runnals, O.J.C.

1959-02-24

The production of alloys of beryllium with one or more of the metals uranium, plutonium, actinium, americium, curium, thorium, and cerium are described. A halide salt of the metal to be alloyed with the beryllium is heated at 1300 deg C in the presence of beryllium to reduce the halide to metal and cause the latter to alloy directly with the beryllium. Although the heavy metal halides are more stable, thermodynamically, than the beryllium halides, the reducing reaction proceeds to completion if the beryllium halide product is continuously removed by vacuum distillation.

The instrumental method of plutonium determination

NASA Astrophysics Data System (ADS)

Knyazev, B. B.; Kazachevskiy, I. V.; Solodukhin, V. P.; Lukashenko, S. N.; Knatova, M. K.; Kashirskiy, V. V.

2003-01-01

A method of direct instrumental determination of plutonium isotopes in soil samples is described. For the method a special program of spectra processing and activity calculation had to be prepared. The detection limit of 239+240Pu in absence of interfering radiation is about 200 Bq/kg (by 3.3σ criteria). Examples are given of the method application for the study of radionuclide soil composition in separate objects of Semipalatinsk Nuclear Test Site (SNTS). It is shown that for different objects under study the correlation degree between plutonium and americium activities may change rather substantially.

The pathology of americium 241.

PubMed

Nilsson, A; Broomé-Karlsson, A

1976-02-01

Male CBA-mice were injected intraperitoneally with different doses of 241Am-citrate (16, 8, 0.4, 0.2, 0.04 muCi/kg). The two highest doses were highly destructive of the haematopoietic tissues, testes and bone tissue. The highest frequency of induced tumours of the skeleton and haematopoietic tissue was found in the 8 muCi group. In the liver, adrenal glands, kidney and heart degenerative lesions were found mainly in the higher dose groups. In the lower dose groups degenerative lesions seemed to appear earlier and at a higher frequency than in the control group.

The efficacies of pure LICAM(C) and DTPA for enhancing the elimination of plutonium-238 and americium-241 from rats after their inhalation as nitrate.

PubMed

Stradling, G N; Stather, J W; Gray, S A; Moody, J C; Ellender, M; Hodgson, A

1989-01-01

After the inhalation of 238Pu and 241Am as nitrate, the repeated administration of DTPA is far superior to that of LICAM(C) for enhancing their elimination from the body. The therapeutic efficacies of these chelating agents are however similar after intravenous injection of 238Pu as citrate. It is concluded that DTPA should remain the agent of choice for treating persons contaminated internally with transportable forms of these actinides.

Observation of beta and X rays with 3-D-architecture silicon microstrip sensors

NASA Astrophysics Data System (ADS)

Kenney, C. J.; Parker, S. I.; Krieger, B.; Ludewigt, B.; Dubbs, T. P.; Sadrozinski, H.

2001-04-01

The first silicon radiation sensors based on the three-dimensional (3-D) architecture have been successfully fabricated. X-ray spectra from iron-55 and americium-241 have been recorded by reading out a 3-D architecture detector via wire bonds to a low-noise, charge-sensitive preamplifier. Using a beta source, coincidences between a 3-D sensor and a plastic scintillator were observed. This is the first observation of ionizing radiation using a silicon sensor based on the 3-D architecture. Details of the apparatus and measurements are described.

Americium behaviour in plastic vessels.

PubMed

Legarda, F; Herranz, M; Idoeta, R; Abelairas, A

2010-01-01

The adsorption of (241)Am dissolved in water in different plastic storage vessels was determined. Three different plastics were investigated with natural and distilled waters and the retention of (241)Am by these plastics was studied. The same was done by varying vessel agitation time, vessel agitation speed, surface/volume ratio of water in the vessels and water pH. Adsorptions were measured to be between 0% and 70%. The adsorption of (241)Am is minimized with no water agitation, with PET or PVC plastics, and by water acidification. Copyright 2009 Elsevier Ltd. All rights reserved.

Chemistry of transuranium elements in salt-base repository

DOE Office of Scientific and Technical Information (OSTI.GOV)

Borkowski, Marian; Reed, Donald T; Lucchini, Jean - Francois

2010-12-02

The mobility and potential release of actinides into the accessible environment continues to be the key performance assessment concern of nuclear repositories. Actinide, in particular plutonium speciation under the wide range of conditions that can exist in the subsurface is complex and depends strongly on the coupled effects of redox conditions, inorganic/organic complexation, and the extent/nature of aggregation. Understanding the key factors that define the potential for actinide migration is, in this context, an essential and critical part of making and sustaining a licensing case for a nuclear repository. Herein we report on recent progress in a concurrent modeling andmore » experimental study to determine the speciation of plutonium, uranium and americium in high ionic strength Na-CI-Mg brines. This is being done as part of the ongomg recertification effort m the Waste Isolation Pilot Plant (WIPP). The oxidation-state specific solubility of actinides were established in brine as function of pC{sub H+}, brine composition and the presence and absence of organic chelating agents and carbonate. An oxidation-state invariant analog approach using Nd{sup 3+} and Th{sup 4+} was used for An{sup 3+} and An{sup 4+} respectively. These results show that organic ligands and hydrolysis are key factors for An(III) solubility, hydrolysis at pC{sub H+} above 8 is predominate for An(IV) and carbonates are the key factor for U(VI) solubility. The effect of high ionic strength and brine components measured in absence of carbonates leads to measurable increased in overall solubility over analogous low ionic strength groundwater. Less is known about the bioreduction of actinides by halo-tolerant microorganisms, but there is now evidence that bioreduction does occur and is analogous, in many ways, to what occurs with soil bacteria. Results of solubility studies that focus on Pitzer parameter corrections, new species (e.g. borate complexation), and the thermodynamic parameters for modeling are discussed.« less

Measured solubilities and speciations from oversaturation experiments of neptunium, plutonium, and americium in UE-25p No. 1 well water from the Yucca Mountain region: Milestone report 3329-WBS1.2.3.4.1.3.1

DOE Office of Scientific and Technical Information (OSTI.GOV)

Nitsche, H.; Roberts, K.; Prussin, T.

1994-04-01

Solubility and speciation are important in understanding aqueous radionuclide transport through the geosphere. They define the source term for transport retardation processes such as sorption and colloid formation. Solubility and speciation data are useful in verifying the validity of geochemical codes that are a part of predictive transport models. Results are presented from solubility and speciation experiments of {sup 237}NpO{sub 2}{sup +}, {sup 239}Pu{sup 4+}, and {sup 241}Am{sup 3+}/Nd{sup 3+} in a modified UE-25p No. 1 groundwater (from the Yucca Mountain region, Nevada, which is being investigated as a potential high-level nuclear waste disposal site) at two different temperatures (25{degree}more » and 60{degree}C) and three pH values (6.0, 7.0, 8.5). The solubility-controlling steady-state solids were identified and the speciation and/or oxidation states present in the supernatant solutions were determined. The neptunium solubility decreased with increasing temperature and pH. Plutonium concentrations significantly decreased with increasing temperature at pH 6 and 7. The concentration at pH 8.5 hardly decreased at all with increasing temperature. At both temperatures the concentrations were highest at pH 8.5, lowest at pH 7, and in between at pH 6. For the americium/neodymium solutions, the solubility decreased significantly with increasing temperature and increased somewhat with increasing pH.« less

Disposition of americium-241 oxide following inhalation by beagles

DOE Office of Scientific and Technical Information (OSTI.GOV)

Craig, D.K.; Park, J.F.; Powers, G.J.

1979-06-01

The disposition of americium-241 in beagles was followed for up to 810 days after a single inhalation exposure to /sup 241/AmO/sub 2/ aerosols having an activity median aerodynamic diameter (AMAD) of 1.3 ..mu..m and a geometric standard deviation 8GSD) of 1.8 for medium (approx. 40 nCi/liter) and high (approx. 340 nCi/liter) concentrations. At low concentrations (< 1 nCi/liter), the aerosols were smaller (AMAD approx. 0.6 ..mu..m) and the distribution broader (GSD approx. 2.6). Excreta were analyzed for up to 30 days postexposure and where appropriate, during the last week before sacrifice. Tissue analyses for /sup 241/Am were conducted on groupsmore » of three dogs sacrificed 10, 30, 90, 270, and 810 days postexposure. Forty percent of the final body burden of /sup 241/Am was located in tissues other than the lung parenchyma by 10 days postexposure and only 6% remained in the lung by 810 days postexposure. Translocation was primarilly to the liver and skeleton, with roughly equal fractions of the final body burden in each at all postexposure sacrifice times. There in the gonads was negligible (< 0.05%) for these dogs. Both the rate of translocation and the organ distribution as a function of time are different from those found in dogs that inhaled /sup 238/PuO/sub 2/ or /sup 239/PuO/sub 2/. Therefore it is not appropriate to use data derived from /sup 239/PuO/sub 2/ experiments or observations to predict the behavior of other transuranic isotopes and elements.« less

Increased retention of americium in kidneys as compared with plutonium in an actinide wound contamination model in the rat.

PubMed

Griffiths, Nina M; Coudert, Sylvie; Molina, Thibaut; Wilk, Jean-Claude; Renault, Daniel; Berard, Philippe; Van der Meeren, Anne

2014-11-01

Americium-241 ((241)Am) presents a potential risk for nuclear industry workers associated with reactor decommissioning and aging combustible materials. The purpose of this study was to investigate Am renal retention after actinide contamination by wounding in the rat. Anesthetized rats were contaminated with Mixed Oxide (MOX) (7.1% Plutonium [Pu] by mass and containing 27% Am as % total alpha activity), Pu or Am nitrate following an incision wound of the hind leg. Times of euthanasia ranged from 2 hours to 5 months after contamination. Pu and Am levels were quantified following radiochemistry and alpha-spectrophotometry. Initial data show that over the experimental period the proportion of Am in kidneys as a fraction of total kidney alpha activity was elevated as compared to MOX powder indicating a specific retention in this organ. The percentage of Pu was similar to the powder. After MOX contamination, kidney to liver ratios appeared to increase more markedly for Am (from 0.2 at 7 days to 0.6 at 90 days) as compared with Pu (0.1 at 7 days to 0.2 at 90 days). In accordance with tissue actinide retention the dose from Am to the kidney increases with time. For comparison, the ratio of estimated equivalent doses due to Am to kidney is 1.5-fold greater than for Pu (around 90 versus 60 mSv). After actinide contamination of wounds, Am is concentrated in the kidneys as compared to Pu leading to potential exposure of renal tissue to both alpha particles and gamma radiation.

A rapid method for the sequential separation of polonium, plutonium, americium and uranium in drinking water.

PubMed

Lemons, B; Khaing, H; Ward, A; Thakur, P

2018-06-01

A new sequential separation method for the determination of polonium and actinides (Pu, Am and U) in drinking water samples has been developed that can be used for emergency response or routine water analyses. For the first time, the application of TEVA chromatography column in the sequential separation of polonium and plutonium has been studied. This method utilizes a rapid Fe +3 co-precipitation step to remove matrix interferences, followed by plutonium oxidation state adjustment to Pu 4+ and an incubation period of ~ 1 h at 50-60 °C to allow Po 2+ to oxidize to Po 4+ . The polonium and plutonium were then separated on a TEVA column, while separation of americium from uranium was performed on a TRU column. After separation, polonium was micro-precipitated with copper sulfide (CuS), while actinides were micro co-precipitated using neodymium fluoride (NdF 3 ) for counting by the alpha spectrometry. The method is simple, robust and can be performed quickly with excellent removal of interferences, high chemical recovery and very good alpha peak resolution. The efficiency and reliability of the procedures were tested by using spiked samples. The effect of several transition metals (Cu 2+ , Pb 2+ , Fe 3+ , Fe 2+ , and Ni 2+ ) on the performance of this method were also assessed to evaluate the potential matrix effects. Studies indicate that presence of up to 25 mg of these cations in the samples had no adverse effect on the recovery or the resolution of polonium alpha peaks. Copyright © 2018 Elsevier Ltd. All rights reserved.

Method of making alloys of beryllium with plutonium and the like

DOEpatents

Runnals, O J.C.

1959-02-24

The production or alloys of beryllium with one or more of the metals uranium, plutonium, actinium, americium, curium, thorium, and cerium is described. A halide salt or the metal to be alloyed with the beryllium is heated at l3O0 deg C in the presence of beryllium to reduce the halide to metal and cause the latter to alloy directly with the beryllium. Although the heavy metal halides are more stable, thermodynamically, than the beryllium halides, the reducing reaction proceeds to completion if the beryllium halide product is continuously removed by vacuum distillation.

An arm phantom for in vivo determination of Americium-241 in bone

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kephart, G.S.; Palmer, H.E.

1988-04-01

The focus of this research has been to construct a realistic arm phantom as a calibration tool in estimation of /sup 241/Am in the bone. The United States Transuranium Registry (USTR), through its program of whole body donations, continues to provide data on transuranic incorporation in man that would not otherwise be readily available (Norwood 1972; Breitenstein 1981; Swint, et al. 1985). This project uses well-characterized human bones loaned by the USTR for the construction of realistic phantoms for improvement of whole-body counter calibrations. 27 refs., 2 figs., 4 tabs.

Removal of actinide elements from liquid scintillation cocktail wastes using liquid-liquid extraction and demulsification techniques

DOE Office of Scientific and Technical Information (OSTI.GOV)

Foltz, K.; Landsberger, S.; Srinivasan, B.

1994-12-31

A method for the separation of radionuclides with Z greater than 88, from lower-level radioactive wastes (liquid scintillation cocktail or LSC wastes), is described. The method is liquid-liquid extraction (LLX) and demulsification. The actinide elements are removed from the LSC wastes by extraction into an aqueous phase after the cocktail has been demulsified. The aqueous and organic phases are separated, then the wastes type remaining may be incinerated. Future experiments will be performed to study the effects of pH and temperature and to extend the study to wastes containing americium.

Schubert Review 2017 2-page summary of AmBe project

DOE Office of Scientific and Technical Information (OSTI.GOV)

Schmidt, A.

2017-04-04

Accelerator-based neutron sources to replace Americium Beryllium (AmBe) radiological sources used for oil well logging are needed for safety and security purposes. DT neutron generators have successfully been used in the past for some measurements, but are less sensitive to rock porosity than the AmBe spectrum is. Additionally, the well-logging industry has decades of data calibrated to the AmBe neutron spectrum. Ideally, if this industry were required to use an accelerator source, they would like a similar neutron spectrum to the AmBe source, with a yield of at least 1×10 7 n/s.

Dissolution of spent nuclear fuel in carbonate-peroxide solution

NASA Astrophysics Data System (ADS)

Soderquist, Chuck; Hanson, Brady

2010-01-01

This study shows that spent UO2 fuel can be completely dissolved in a room temperature carbonate-peroxide solution apparently without attacking the metallic Mo-Tc-Ru-Rh-Pd fission product phase. In parallel tests, identical samples of spent nuclear fuel were dissolved in nitric acid and in an ammonium carbonate, hydrogen peroxide solution. The resulting solutions were analyzed for strontium-90, technetium-99, cesium-137, europium-154, plutonium, and americium-241. The results were identical for all analytes except technetium, where the carbonate-peroxide dissolution had only about 25% of the technetium that the nitric acid dissolution had.

A combined Cyanex-923/HEH[EHP]/Dodecane solvent for recovery of transuranic elements from used nuclear fuel

DOE Office of Scientific and Technical Information (OSTI.GOV)

Johnson, A.; Nash, K.L.

2013-07-01

The separation of minor actinides from fission product lanthanides remains a primary challenge for enabling the recycle of used nuclear fuel. To minimize the complexity of materials handling, combining extractant processes has become an increasingly attractive option. Unfortunately, combined processes sometimes suffer reduced utility due to strong dipole-dipole interactions between the extractants. The results reported here describe a system based on a combination of commercially available extractants Cyanex-923 and HEH[EHP]. In contrast to other combined extractant systems, these extractant molecules exhibit comparatively weak interactions, reducing the impact of secondary interactions. In this process, mixtures containing equal ratios of Cyanex-923 andmore » HEH[EHP] were seen to co-extract americium and the lanthanides from nitric acid solutions. Stripping of An(III) was effectively achieved through contact with an aqueous phase comprised of glycine (for pH control) and a polyamino-poly-carboxylate stripping reagent that selectively removes An(III) from the extractant phase. The lanthanides can then be stripped from the loaded organic phase contacting with high nitric acid concentrations. Extraction of fission products zirconium and molybdenum was also investigated and potential strategies for their management have been identified. The work presented demonstrates the feasibility of combining Cyanex-923 and HEH[EHP] for separating and recovering the transuranic elements from the Ln(III). (authors)« less

DISSOLVED CONCENTRATION LIMITS OF RADIOACTIVE ELEMENTS

DOE Office of Scientific and Technical Information (OSTI.GOV)

P. Bernot

The purpose of this study is to evaluate dissolved concentration limits (also referred to as solubility limits) of elements with radioactive isotopes under probable repository conditions, based on geochemical modeling calculations using geochemical modeling tools, thermodynamic databases, field measurements, and laboratory experiments. The scope of this activity is to predict dissolved concentrations or solubility limits for elements with radioactive isotopes (actinium, americium, carbon, cesium, iodine, lead, neptunium, plutonium, protactinium, radium, strontium, technetium, thorium, and uranium) relevant to calculated dose. Model outputs for uranium, plutonium, neptunium, thorium, americium, and protactinium are provided in the form of tabulated functions with pH andmore » log fCO{sub 2} as independent variables, plus one or more uncertainty terms. The solubility limits for the remaining elements are either in the form of distributions or single values. Even though selection of an appropriate set of radionuclides documented in Radionuclide Screening (BSC 2002 [DIRS 160059]) includes actinium, transport of Ac is not modeled in the total system performance assessment for the license application (TSPA-LA) model because of its extremely short half-life. Actinium dose is calculated in the TSPA-LA by assuming secular equilibrium with {sup 231}Pa (Section 6.10); therefore, Ac is not analyzed in this report. The output data from this report are fundamental inputs for TSPA-LA used to determine the estimated release of these elements from waste packages and the engineered barrier system. Consistent modeling approaches and environmental conditions were used to develop solubility models for the actinides discussed in this report. These models cover broad ranges of environmental conditions so they are applicable to both waste packages and the invert. Uncertainties from thermodynamic data, water chemistry, temperature variation, and activity coefficients have been quantified or otherwise addressed.« less

Distribution coefficients (Kd's) for use in risk assessment models of the Kara Sea.

PubMed

Carroll, J; Boisson, F; Teyssie, J L; King, S E; Krosshavn, M; Carroll, M L; Fowler, S W; Povinec, P P; Baxter, M S

1999-07-01

As a prerequisite for most evaluations of radionuclide transport pathways in marine systems, it is necessary to obtain basic information on the sorption potential of contaminants onto particulate matter. Kd values for use in modeling radionuclide dispersion in the Kara Sea have been determined as part of several international programs addressing the problem of radioactive debris residing in Arctic Seas. Field and laboratory Kd experiments were conducted for the following radionuclides associated with nuclear waste: americium, europium, plutonium, cobalt, cesium and strontium. Emphasis has been placed on two regions in the Kara Sea: (i) the Novaya Zemlya Trough (NZT) and (ii) the mixing zones of the Ob and Yenisey Rivers (RMZ). Short-term batch Kd experiments were performed at-sea on ambient water column samples and on samples prepared both at-sea and in the laboratory by mixing filtered bottom water with small amounts of surficial bottom sediments (particle concentrations in samples = 1-30 mg/l). Within both regions, Kd values for individual radionuclides vary over two to three orders of magnitude. The relative particle affinities for radionuclides in the two regions are americium approximately equal to europium > plutonium > cobalt > cesium > strontium. The values determined in this study agree with minimum values given in the IAEA Technical Report [IAEA, 1985. Sediment Kd's and Concentration Factors for Radionuclides in the Marine Environment. Technical Report No. 247. International Atomic Energy Agency, Vienna.]. Given the importance of Kd's in assessments of critical transport pathways for radionuclide contaminants, we recommend that Kd ranges of values for specific elements rather than single mean values be incorporated into model simulations of radionuclide dispersion.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rogers, D.M.; Coggins, T.L.; Marsh, J.

Numerous efforts are funded by US agencies (DOE, DoD, DHS) for development of novel radiation sensing and measurement systems. An effort has been undertaken to develop a flexible shielding system compatible with a variety of sources (beta, X-ray, gamma, and neutron) that can be highly characterized using conventional radiation detection and measurement systems. Sources available for use in this system include americium-beryllium (AmBe), plutonium-beryllium (PuBe), strontium-90 (Sr-90), californium-252 (Cf-252), krypton-85 (Kr-85), americium-241 (Am-241), and depleted uranium (DU). Shielding can be varied by utilization of materials that include lexan, water, oil, lead, and polyethylene. Arrangements and geometries of source(s) and shieldingmore » can produce symmetrical or asymmetrical radiation fields. The system has been developed to facilitate accurately repeatable configurations. Measurement positions are similarly capable of being accurately re-created. Stand-off measurement positions can be accurately re-established using differential global positioning system (GPS) navigation. Instruments used to characterize individual measurement locations include a variety of sodium iodide (NaI(Tl)) (3 x 3 inch, 4 x 4 x 16 inch, Fidler) and lithium iodide (LiI(Eu)) detectors (for use with multichannel analyzer software) and detectors for use with traditional hand held survey meters such as boron trifluoride (BF{sub 3}), helium-3 ({sup 3}He), and Geiger-Mueller (GM) tubes. Also available are Global Dosimetry thermoluminescent dosimeters (TLDs), CR39 neutron chips, and film badges. Data will be presented comparing measurement techniques with shielding/source configurations. The system is demonstrated to provide a highly functional process for comparison/characterization of various detector types relative to controllable radiation types and levels. Particular attention has been paid to use of neutron sources and measurements. (authors)« less

An aerial radiological survey of the Nevada Test Site

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hendricks, T J; Riedhauser, S R

1999-12-01

A team from the Remote Sensing Laboratory conducted an aerial radiological survey of the US Department of Energy's Nevada Test Site including three neighboring areas during August and September 1994. The survey team measured the terrestrial gamma radiation at the Nevada Test Site to determine the levels of natural and man-made radiation. This survey included the areas covered by previous surveys conducted from 1962 through 1993. The results of the aerial survey showed a terrestrial background exposure rate that varied from less than 6 microroentgens per hour (mR/h) to 50 mR/h plus a cosmic-ray contribution that varied from 4.5 mR/hmore » at an elevation of 900 meters (3,000 feet) to 8.5 mR/h at 2,400 meters (8,000 feet). In addition to the principal gamma-emitting, naturally occurring isotopes (potassium-40, thallium-208, bismuth-214, and actinium-228), the man-made radioactive isotopes found in this survey were cobalt-60, cesium-137, europium-152, protactinium-234m an indicator of depleted uranium, and americium-241, which are due to human actions in the survey area. Individual, site-wide plots of gross terrestrial exposure rate, man-made exposure rate, and americium-241 activity (approximating the distribution of all transuranic material) are presented. In addition, expanded plots of individual areas exhibiting these man-made contaminations are given. A comparison is made between the data from this survey and previous aerial radiological surveys of the Nevada Test Site. Some previous ground-based measurements are discussed and related to the aerial data. In regions away from man-made activity, the exposure rates inferred from the gamma-ray measurements collected during this survey agreed very well with the exposure rates inferred from previous aerial surveys.« less

Radionuclides in shallow groundwater at Solid Waste Storage Area 5 North, Oak Ridge National Laboratory

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ashwood, T.L.; Marsh, J.D. Jr.

1994-04-01

This report presents a compilation of groundwater monitoring data from Solid Waste Storage Area (SWSA) 5 North at Oak Ridge National Laboratory (ORNL) between November 1989 and September 1993. Monitoring data were collected as part of the Active Sites Environmental Monitoring Program that was implemented in 1989 in response to DOE Order 5820.2A. SWSA 5 North was established for the retrievable storage of transuranic (TRU) wastes in 1970. Four types of storage have been used within SWSA 5 North: bunkers, vaults, wells, and trenches. The fenced portion of SWSA 5 North covers about 3.7 ha (9 acres) in the Whitemore » Oak Creek watershed south of ORNL. The area is bounded by White Oak Creek and two ephemeral tributaries of White Oak Creek. Since 1989, groundwater has been monitored in wells around SWSA 5 North. During that time, elevated gross alpha contamination (reaching as high as 210 Bq/L) has consistently been detected in well 516. This well is adjacent to burial trenches in the southwest corner of the area. Water level measurements in wells 516 and 518 suggest that water periodically inundates the bottom of some of those trenches. Virtually all of the gross alpha contamination is generated by Curium 244 and Americium 241. A special geochemical investigation of well 516 suggests that nearly all of the Curium 44 and Americium 241 is dissolved or associated with dissolved organic matter. These are being transported at the rate of about 2 m/year from the burial trenches, through well 516, to White Oak Creek, where Curium 244 has been detected in a few bank seeps. Concentrations at these seeps are near detection levels (<1 Bq/L).« less

Spatial analysis of plutonium-239 + 240 and Americium-241 in soils around Rocky Flats, Colorado

DOE Office of Scientific and Technical Information (OSTI.GOV)

Litaor, M.I.

1995-05-01

Plutonium and american contamination of soils around Rocky Flats, Colorado resulted from past outdoor storage practices. Four previous studies produce four different Pu isopleth maps. Spatial estimation techniques were not used in the construction of these maps and were also based on an extremely small number of soil samples. The purpose of this study was to elucidate the magnitude of Pu-239 + 240 and Am-241 dispersion in the soil environment east of Rocky Flats using robust spatial estimation techniques. Soils were sampled from 118 plots of 1.01 and 4.05 ha by compositing 25 evenly spaced samples in each plot frommore » the top 0.64 cm. Plutonium-239 + 240 activity ranged from 1.85 to 53 560 Bq/kg with a mean of 1924 Bq/kg and a standard deviation of 6327 Bq/kg. Americium-241 activity ranged from 0.18 to 9990 Bq/kg with a mean of 321 Bq/kg and a standard deviation of 1143 Bq/kg. Geostatistical techniques were used to model the spatial dependency and construct isopleth maps showing Pu-239 + 240 and Am-241 distribution. The isopleth configuration was consistent with the hypothesis that the dominant dispersal mechanism of Pu-239 + 240 was wind dispersion from west to east. The Pu-239 + 240 isopleth map proposed to this study differed significantly in the direction and distance of dispersal from the previously published maps. This ispleth map as well as the Am-241 map should be used as the primary data for future risk assessment associated with public exposure to Pu-239 + 240 and Am-241. 37 refs., 7 figs., 2 tabs.« less

Adsorption and dissociation of molecular hydrogen on the (0001) surface of double hexagonal close packed americium

NASA Astrophysics Data System (ADS)

Dholabhai, P. P.; Ray, A. K.

2009-01-01

Hydrogen molecule adsorption on the (0001) surface of double hexagonal packed americium has been studied in detail within the framework of density functional theory using a full-potential all-electron linearized augmented plane wave plus local orbitals method (FP-L/APW+lo). Weak molecular hydrogen adsorptions were observed. Adsorption energies were optimized with respect to the distance of the adsorbates from the surface for three approach positions at three adsorption sites, namely t1 (one-fold top), b2 (two-fold bridge), and h3 (three-fold hollow) sites. Adsorption energies were computed at the scalar-relativistic level (no spin-orbit coupling NSOC) and at the fully relativistic level (with spin-orbit coupling SOC). The most stable configuration corresponds to a horizontal adsorption with the molecular approach being perpendicular to a lattice vector. The surface coverage is equivalent to one-fourth of a monolayer (ML), with the adsorption energies at the NSOC and SOC theoretical levels being 0.0997 eV and 0.1022 eV, respectively. The respective distance of the hydrogen molecule from the surface and hydrogen-hydrogen distance was found to be 2.645 Å and 0.789 Å, respectively. The work functions decreased and the net magnetic moments remained almost unchanged in all cases compared with the corresponding quantities of bare dhcp Am (0001) surface. The adsorbate-substrate interactions have been analyzed in detail using the partial charges inside the muffin-tin spheres, difference charge density distributions, and the local density of states. The effects of adsorption on the Am 5f electron localization-delocalization characteristics have been discussed. Reaction barrier for the dissociation of hydrogen molecule has been presented.

Depth profiling of Pu, 241Am and 137Cs in soils from southern Belarus measured by ICP-MS and alpha and gamma spectrometry.

PubMed

Boulyga, Sergei F; Zoriy, Myroslav; Ketterer, Michael E; Becker, J Sabine

2003-08-01

The depth distribution of plutonium, americium, and 137Cs originating from the 1986 accident at the Chernobyl Nuclear Power Plant (NPP) was investigated in several soil profiles in the vicinity from Belarus. The vertical migration of transuranic elements in soils typical of the 30 km relocation area around Chernobyl NPP was studied using inductively coupled plasma mass spectrometry (ICP-MS), alpha spectrometry, and gamma spectrometry. Transuranic concentrations in upper soil layers ranged from 6 x 10(-12) g g(-1) to 6 x 10(-10) g g(-1) for plutonium and from 1.8 x 10(-13) g g(-1) to 1.6 x 10(-11) g g(-1) for americium. These concentrations correspond to specific activities of (239+240)Pu of 24-2400 Bq kg(-1) and specific activity of 241Am of 23-2000 Bq kg(-1), respectively. Transuranics in turf-podzol soil migrate slowly to the deeper soil layers, thus, 80-95%, of radionuclide inventories were present in the 0-3 cm intervals of turf-podzol soils collected in 1994. In peat-marsh soil migration processes occur more rapidly than in turf-podzol and the maximum concentrations are found beneath the soil surface (down to 3-6 cm). The depth distributions of Pu and Am are essentially identical for a given soil profile. (239+240)Pu/137Cs and 241Am/137Cs activity ratios vary by up to a factor of 5 at some sites while smaller variations in these ratios were observed at a site close to Chernobyl, suggesting that 137Cs is dominantly particle associated close to Chernobyl but volatile species of 137Cs are of relatively greater importance at the distant sites.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Herring, G. M.; Vaughan, Janet; Williamson, Margaret

Characteristics of bone surfaces are discussed in relation to the uptake of bone-seeking isotopes. The alkaline earths are concentrated behind the osteoid border of active surfaces. Yttrium, americium, and plutonium are concentrated on quiescent and resorbing surfaces; traces only occur in and beneath the osteoid border. In view of evidence of mucoproteins at sites where the latter elemerts are found in concentration, a separation of the mucoproteins in cortical bone was undertaken. Mucosubstances have been isolated which give the same reaction with certain reagents as the bone surfaces in question. One of these, a sialoprotein, might be expected, in viewmore » of its acidic nature, to be capable of metal binding.« less

Historical Development of the U.S. Geological Survey Hydrologic Monitoring and Investigative Programs at the Idaho National Engineering and Environmental Laboratory, Idaho, 1949 to 2001

DTIC Science & Technology

2005-01-01

Cesium- 137 , Cobalt-60, and Chromium-51 ………………………………………… 12 Plutonium-238, Plutonium-239, -240 (undivided), and Americium-241 ……………… 12 Iodine-129...1992) presented water-level data from the ESRPA collected from 1983 through 1990 from 137 wells. At the end of 2000, water levels in 203 aquifer and...Cesium- 137 , Cobalt-60, and Chromium-51 The USGS has routinely monitored ground water at the INEEL for gamma radiation since 1962. Gamma

Detecting Illicit Trafficking

DTIC Science & Technology

2001-09-01

n , p ’b 9 MeV and up activ.,7.13 s C0 ’Cl( n ,I : Ca thermal prompt Ci 35Cl ( n , n 𔃾 C:)3Ci 3 MeV and up prompt CI 7Ci( n , p )yS 14 MeV activ.,4.9 min 377 ...Octogene 3.95 ppt/ 3x 10- 9 9,1 376 Table 2. Elementary composition of some CW agents (atom number/molecule). Agent Cl P As S F 0 N C H S-Mustard (HD) 2 1...types of sources are used: 252Cf that decays by spontaneous fission and Be(a, n ) sources, where as an a emitter americium, or plutonium,

Effect of ethanol on the retention of americium-241 in the baboon liver.

PubMed

Cohen, N; Antonelli, R; Lo Sasso, T; Wrenn, M E

1978-01-01

The oral administration of ethyl alcohol enhanced the excretion of 241Am from the liver of a baboon by 2.5 times that of a control animal. After ethanol administration, increases in the total content of 241Am excreted in feces were accompanied by corresponding increases in fecal volumes, although administration of nonalcoholic cathartics would not be expected to produce a similar effect. The effectiveness of ethanol as a decorporating agent may result from its ability to mobilize intracellularly bound 241Am from the liver, thereby making the nuclide more available for metabolic secretory mechanisms occurring via liver-bile-fecal route.

Hole defects in molecular beam epitaxially grown p-GaAs introduced by alpha irradiation

NASA Astrophysics Data System (ADS)

Goodman, S. A.; Auret, F. D.; Meyer, W. E.

1994-01-01

Epitaxial aluminum Schottky barrier diodes on molecular beam epitaxially grown p-GaAs with a free carrier density of 2×1016 cm-3 were irradiated with alpha particles at room temperature using an americium-241 (Am-241) radio nuclide. For the first time, the radiation induced hole defects are characterized using conventional deep level transient spectroscopy (DLTS). The introduction rates and DLTS ``signatures'' of three prominent radiation induced defects Hα1, Hα4, and Hα5, situated 0.08, 0.20, and 0.30 eV above the valence band, respectively, are calculated and compared to those of similar defects introduced during electron irradiation.

Characteristics of Chernobyl-derived radionuclides in particulate form in surface waters in the exclusion zone around the Chernobyl Nuclear Power Plant

NASA Astrophysics Data System (ADS)

Matsunaga, Takeshi; Ueno, Takashi; Amano, Hikaru; Tkatchenko, Y.; Kovalyov, A.; Watanabe, Miki; Onuma, Yoshikazu

1998-12-01

The distribution of Chernobyl-derived radionuclides in river and lake water bodies at 6-40 km from the Chernobyl Nuclear Power Plant was studied. Current levels of radionuclides (Cesium-137, Strontium-90, Plutonium, Americium and Curium isotopes) in water bodies and their relation to the ground contamination are presented. The investigation of the radionuclide composition of aqueous and ground contamination revealed that radionuclides on suspended solids (particulate form) originate mainly from the erosion of the contaminated surface soil layer in the zone. Apparent distribution ratios between particulate and dissolved forms are compared to known distribution coefficients.

The New Element Berkelium (Atomic Number 97)

DOE R&D Accomplishments Database

Seaborg, G. T.; Thompson, S. G.; Ghiorso, A.

1950-04-26

An isotope of the element with atomic number 97 has been discovered as a product of the helium-ion bombardment of americium. The name berkelium, symbol Bk, is proposed for element 97. The chemical separation of element 97 from the target material and other reaction products was made by combinations of precipitation and ion exchange adsorption methods making use of its anticipated (III) and (IV) oxidation states and its position as a member of the actinide transition series. The distinctive chemical properties made use of in its separation and the equally distinctive decay properties of the particular isotope constitute the principal evidence for the new element.

Studies on transformations of plutonium-239 and americium-241 in three major Indian soils.

PubMed

Vyas, B N; Mistry, K B

1984-01-13

These studies were carried out to elucidate the behaviour of 239Pu and and 241Am in three major soil groups of India, namely oxisol, vertisol-pellustert and entisol-haplaquent, over extended periods up to 400 days. The influences of soil characteristics, addition of organic matter and the chemical form of the radionuclides added to soils were investigated. A large fraction, ranging from 60 to 90% of the soluble radionuclides added as nitrates, underwent rapid conversion to precipitated hydrous oxides and hydroxides (0.3 M sodium citrate-dithionite extracts). At 3 h after contamination, ion-exchangeable forms (0.1 M MgCl2 extracts) contained low levels of total added Pu (0.7 to 19.1%) and from 0.1 to 2.8% of total Am. These levels decreased further with increasing periods of incubation of up to 400 days. In contrast, on addition of chelated forms of radionuclides (as DTPA and EDTA complexes) up to 85% of total Pu, and about 50% of total Am were associated with 0.1 M MgCl2 extracts 3 h post-contamination and significant amounts were extractable when maintained over extended periods of incubation of up to 400 days. The levels of Pu and Am associated with organic-bound forms (0.1 M NaOH extracts) did not show consistent trends, although in all three soil types the contents of these radionuclides in the insoluble residue fraction (including refractory compounds) generally increased with time of incubation.

Detection of Alpha Particles and Low Energy Gamma Rays by Thermo-Bonded Micromegas in Xenon Gas

NASA Astrophysics Data System (ADS)

Wei, Yuehuan; Guan, Liang; Zhang, Zhiyong; Lin, Qing; Wang, Xiaolian; Ni, Kaixuan; Zhao, Tianchi

2013-08-01

Micromegas is a type of micro-pattern gaseous detector currently under R&D for applications in rare event search experiments. Here we report the performance of a Micromegas structure constructed with a micromesh thermo-bonded to a readout plane, motivated by its potential application in two-phase xenon detectors for dark matter and neutrinoless double beta decay experiments. The study is carried out in pure xenon at room temperature. Measurements with alpha particles from the Americium-241 source showed that gas gains larger than 200 can be obtained at xenon pressure up to 3 atm. Gamma rays down to 8 keV were observed with such a device.

[Carcinogenic efficacy of the transuranium elements americium-241 and curium-244].

PubMed

Rudnitskaia, E I

1984-01-01

Albino female rats were used in the experiments. After a single intraperitoneal administration of 241Am and 244Cm chloride is doses ranging from 0.37 to 185 kBq/kg (14 doses were used) it was established that the doses applied had different effect on the average life of animals. The largest doses shortened and the lowest increased the life span of experimental animals as compared to the controls. The carcinogenic effect of the studied radionuclides and the development of malignant tumors were detected at sufficiently low doses absorbed. Malignant tumors developed in the experimental and control animals were different not only in their incidence but also their localization and spectrum.

Alpha-ray detection with a MgB 2 transition edge sensor

NASA Astrophysics Data System (ADS)

Okayasu, S.; Katagiri, M.; Hojou, K.; Morii, Y.; Miki, S.; Shimakage, H.; Wang, Z.; Ishida, T.

2008-09-01

We have been investigating for neutron detection with the MgB 2 transition edge sensor (TES). For the purpose, we have been developing a low noise measurement system for the detection. To confirm the performance of the detecting sensor, alpha ray detection from an americium-241 ( 241Am) alpha-ray source was achieved. A short microfabricated sample with 10 μm length and 1 μm width is used to improve the S/N ratio. The detection is achieved under a constant current condition in the range between 1 and 6 μA bias current, and the resistivity changes at the sample due to the alpha ray irradiation is detected just on the transition edge.

Effect of alpha-particle irradiation on the electrical properties of n-type Ge

NASA Astrophysics Data System (ADS)

Roro, K. T.; Janse van Rensburg, P. J.; Auret, F. D.; Coelho, S.

2009-12-01

Deep-level transient spectroscopy was used to investigate the effect of alpha particle irradiation on the electrical properties of n-type Ge. The samples were irradiated with alpha particles at room temperature using an americium-241 (Am-241) radionuclide source. The main defects introduced were found to be electron traps with energy levels at EC-0.38, EC-0.21, EC-0.20, EC-0.15, and EC-0.10 eV, respectively. The main defects in alpha particle irradiation are similar to those introduced by MeV electron irradiation, where the main defect is the E-center. A quadratic increase in concentration as a function of dose is observed.

Technical basis for internal dosimetry at Hanford

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sula, M.J.; Carbaugh, E.H.; Bihl, D.E.

1991-07-01

The Hanford Internal Dosimetry Program, administered by Pacific Northwest Laboratory for the US Department of Energy, provides routine bioassay monitoring for employees who are potentially exposed to radionuclides in the workplace. This report presents the technical basis for routine bioassay monitoring and the assessment of internal dose at Hanford. The radionuclides of concern include tritium, corrosion products ({sup 58}Co, {sup 60}Co, {sup 54}Mn, and {sup 59}Fe), strontium, cesium, iodine, europium, uranium, plutonium, and americium,. Sections on each of these radionuclides discuss the sources and characteristics; dosimetry; bioassay measurements and monitoring; dose measurement, assessment, and mitigation and bioassay follow-up treatment. 78more » refs., 35 figs., 115 tabs.« less

Technical basis for internal dosimetry at Hanford

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sula, M.J.; Carbaugh, E.H.; Bihl, D.E.

1989-04-01

The Hanford Internal Dosimetry Program, administered by Pacific Northwest Laboratory for the US Department of Energy, provides routine bioassay monitoring for employees who are potentially exposed to radionuclides in the workplace. This report presents the technical basis for routine bioassay monitoring and the assessment of internal dose at Hanford. The radionuclides of concern include tritium, corrosion products (/sup 58/Co, /sup 60/Co, /sup 54/Mn, and /sup 59/Fe), strontium, cesium, iodine, europium, uranium, plutonium, and americium. Sections on each of these radionuclides discuss the sources and characteristics; dosimetry; bioassay measurements and monitoring; dose measurement, assessment, and mitigation; and bioassay follow-up treatment. 64more » refs., 42 figs., 118 tabs.« less

Radioactivity of Consumer Products

NASA Astrophysics Data System (ADS)

Peterson, David; Jokisch, Derek; Fulmer, Philip

2006-11-01

A variety of consumer products and household items contain varying amounts of radioactivity. Examples of these items include: FiestaWare and similar glazed china, salt substitute, bananas, brazil nuts, lantern mantles, smoke detectors and depression glass. Many of these items contain natural sources of radioactivity such as Uranium, Thorium, Radium and Potassium. A few contain man-made sources like Americium. This presentation will detail the sources and relative radioactivity of these items (including demonstrations). Further, measurements of the isotopic ratios of Uranium-235 and Uranium-238 in several pieces of china will be compared to historical uses of natural and depleted Uranium. Finally, the presenters will discuss radiation safety as it pertains to the use of these items.

Coder’s Manual: A Guide to TEPIAC Documentation.

DTIC Science & Technology

1977-07-01

Po Polonium Am Americium Hg Mercury Pr Praseodymium *Ar Argon (Hydrargyrum) Pt Platinum (also A) Ho Holmium Pu Plutonium *As Arsenic *1 Iodine Ra...Er 20 3 208 D ChD2 110 F F 2 Fe (FeF 21 209 E C 6H1 5ErO1 2S 3[Er(C 2 HSO 4)3] III G GaO4P [GaPO4] 210 F CH3 F 112 H 1iNO 212 G C8 H20Ge [Ge(C 2 H 5...Fluidity, 69 Heat conductance (contact), 62 Fluidized bed, 27 Heat conduction, 57 Fluorescence, 125 Heat conductivity, 57 Food products, 31 Heat content

Americium As A Potential Power Source For Space Missions

NASA Astrophysics Data System (ADS)

Cordingley, Leon; Rice, Tom; Sarsfield, Mark J.; Stephenson, Keith; Tinsley, Tim

2011-10-01

Electrical power sources used in outer planet missions are a key enabling technology for data acquisition and communications. Power sources generate electricity from the thermal energy from alpha decay of the radioisotope 238Pu via thermoelectric conversion. Production of 238Pu requires specialist facilities including a nuclear reactor and reprocessing plants that are expensive to build and operate, so naturally, a more economical alternative is attractive to the industry. Within Europe 241Am is a feasible alternative to 238Pu that can provide a heat source for radioisotope thermoelectric generators (RTGs) and radioisotope heating units (RHUs). Whilst there are implications associated with the differences between 238Pu and 241Am, these technological challenges are surmountable.

Review of the transport of selected radionuclides in the interim risk assessment for the Radioactive Waste Management Complex, Waste Area Group 7 Operable Unit 7-13/14, Idaho National Engineering and Environmental Laboratory, Idaho

USGS Publications Warehouse

Rousseau, Joseph P.; Landa, Edward R.; Nimmo, John R.; Cecil, L. DeWayne; Knobel, LeRoy L.; Glynn, Pierre D.; Kwicklis, Edward M.; Curtis, Gary P.; Stollenwerk, Kenneth G.; Anderson, Steven R.; Bartholomay, Roy C.; Bossong, Clifford R.; Orr, Brennon R.

2005-01-01

The U.S. Department of Energy (DOE) requested that the U.S. Geological Survey conduct an independent technical review of the Interim Risk Assessment (IRA) and Contaminant Screening for the Waste Area Group 7 (WAG-7) Remedial Investigation, the draft Addendum to the Work Plan for Operable Unit 7-13/14 WAG-7 comprehensive Remedial Investigation and Feasibility Study (RI/FS), and supporting documents that were prepared by Lockheed Martin Idaho Technologies, Inc. The purpose of the technical review was to assess the data and geotechnical approaches that were used to estimate future risks associated with the release of the actinides americium, uranium, neptunium, and plutonium to the Snake River Plain aquifer from wastes buried in pits and trenches at the Subsurface Disposal Area (SDA). The SDA is located at the Radioactive Waste Management Complex in southeastern Idaho within the boundaries of the Idaho National Engineering and Environmental Laboratory. Radionuclides have been buried in pits and trenches at the SDA since 1957 and 1952, respectively. Burial of transuranic wastes was discontinued in 1982. The five specific tasks associated with this review were defined in a ?Proposed Scope of Work? prepared by the DOE, and a follow-up workshop held in June 1998. The specific tasks were (1) to review the radionuclide sampling data to determine how reliable and significant are the reported radionuclide detections and how reliable is the ongoing sampling program, (2) to assess the physical and chemical processes that logically can be invoked to explain true detections, (3) to determine if distribution coefficients that were used in the IRA are reliable and if they have been applied properly, (4) to determine if transport model predictions are technically sound, and (5) to identify issues needing resolution to determine technical adequacy of the risk assessment analysis, and what additional work is required to resolve those issues.

On the use of X-ray absorption spectroscopy to elucidate the structure of lutetium adenosine mono- and triphosphate complexes.

PubMed

Mostapha, S; Berthon, C; Fontaine-Vive, F; Gaysinski, M; Guérin, L; Guillaumont, D; Massi, L; Monfardini, I; Solari, P L; Thomas, O P; Charbonnel, M C; Den Auwer, C

2014-02-01

Although the physiological impact of the actinide elements as nuclear toxicants has been widely investigated for half a century, a description of their interactions with biological molecules remains limited. It is however of primary importance to better assess the determinants of actinide speciation in cells and more generally in living organisms to unravel the molecular processes underlying actinide transport and deposition in tissues. The biological pathways of this family of elements in case of accidental contamination or chronic natural exposure (in the case of uranium rich soils for instance) are therefore a crucial issue of public health and of societal impact. Because of the high chemical affinity of those actinide elements for phosphate groups and the ubiquity of such chemical functions in biochemistry, phosphate derivatives are considered as probable targets of these cations. Among them, nucleotides and in particular adenosine mono- (AMP) and triphosphate (ATP) nucleotides occur in more chemical reactions than any other compounds on the earth's surface, except water, and are therefore critical target molecules. In the present study, we are interested in trans-plutonium actinide elements, in particular americium and curium that are more rarely considered in environmental and bioaccumulation studies than early actinides like uranium, neptunium and plutonium. A first step in this strategy is to work with chemical analogues like lanthanides that are not radioactive and therefore allow extended physical chemical characterization to be conducted that are difficult to perform with radioactive materials. We describe herein the interaction of lutetium(III) with adenosine AMP and ATP. With AMP and ATP, insoluble amorphous compounds have been obtained with molar ratios of 1:2 and 1:1, respectively. With an excess of ATP, with 1:2 molar ratio, a soluble complex has been obtained. A combination of spectroscopic techniques (IR, NMR, ESI-MS, EXAFS) together with quantum chemical calculations has been implemented in order to assess the lutetium coordination arrangement for the two nucleotides. In all the complexes described in the article, the lutetium cation is coordinated by the phosphate groups of the nucleotide plus additional putative water molecules with various tridimensional arrangements. With AMP 1:2 and ATP 1:1 solid-state compounds, polynuclear complexes are assumed to be obtained. In contrast, with ATP 1:2 soluble compound, the Lu coordination sphere is saturated by two ATP ligands, and this favors the formation of a mononuclear complex. In order to further interpret the EXAFS data obtained at the Lu LIII edge, model structures have been calculated for the 1:1 and 1:2 ATP complexes. They are discussed and compared to the EXAFS best fit metrical parameters.

Facility-specific radiation exposure risks and their implications for radiation workers at Department of Energy laboratories

NASA Astrophysics Data System (ADS)

Davis, Adam Christopher

This research develops a new framework for evaluating the occupational risks of exposure to hazardous substances in any setting where As Low As Reasonably Achievable (ALARA) practices are mandated or used. The evaluation is performed by developing a hypothesis-test-based procedure for evaluating the homogeneity of various epidemiological cohorts, and thus the appropriateness of the application of aggregate data-pooling techniques to those cohorts. A statistical methodology is then developed as an alternative to aggregate pooling for situations in which individual cohorts show heterogeneity between them and are thus unsuitable for pooled analysis. These methods are then applied to estimate the all-cancer mortality risks incurred by workers at four Department-of-Energy nuclear weapons laboratories. Both linear, no-threshold and dose-bin averaged risks are calculated and it is further shown that aggregate analysis tends to overestimate the risks with respect to those calculated by the methods developed in this work. The risk estimates developed in Chapter 2 are, in Chapter 3, applied to assess the risks to workers engaged in americium recovery operations at Los Alamos National Laboratory. The work described in Chapter 3 develops a full radiological protection assessment for the new americium recovery project, including development of exposure cases, creation and modification of MCNP5 models, development of a time-and-motion study, and the final synthesis of all data. This work also develops a new risk-based method of determining whether administrative controls, such as staffing increases, are ALARA-optimized. The EPA's estimate of the value of statistical life is applied to these risk estimates to determine a monetary value for risk. The rate of change of this "risk value" (marginal risk) is then compared with the rate of change of workers' compensations as additional workers are added to the project to reduce the dose (and therefore, presumably, risk) to each individual.

A density functional study of atomic hydrogen and oxygen chemisorption on the relaxed (0001) surface of double hexagonal close packed americium

NASA Astrophysics Data System (ADS)

Dholabhai, P. P.; Atta-Fynn, R.; Ray, A. K.

2008-02-01

Ab initio total energy calculations within the framework of density functional theory have been performed for atomic hydrogen and oxygen chemisorption on the (0001) surface of double hexagonal packed americium using a full-potential all-electron linearized augmented plane wave plus local orbitals method. Chemisorption energies were optimized with respect to the distance of the adatom from the relaxed surface for three adsorption sites, namely top, bridge, and hollow hcp sites, the adlayer structure corresponding to coverage of a 0.25 monolayer in all cases. Chemisorption energies were computed at the scalar-relativistic level (no spin-orbit coupling NSOC) and at the fully relativistic level (with spin-orbit coupling SOC). The two-fold bridge adsorption site was found to be the most stable site for O at both the NSOC and SOC theoretical levels with chemisorption energies of 8.204 eV and 8.368 eV respectively, while the three-fold hollow hcp adsorption site was found to be the most stable site for H with chemisorption energies of 3.136 eV at the NSOC level and 3.217 eV at the SOC level. The respective distances of the H and O adatoms from the surface were found to be 1.196 Åand 1.164 Å. Overall our calculations indicate that chemisorption energies in cases with SOC are slightly more stable than the cases with NSOC in the 0.049 0.238 eV range. The work functions and net magnetic moments respectively increased and decreased in all cases compared with the corresponding quantities of bare dhcp Am (0001) surface. The partial charges inside the muffin-tins, difference charge density distributions, and the local density of states have been used to analyze the Am-adatom bond interactions in detail. The implications of chemisorption on Am 5f electron localization-delocalization are also discussed.

University of Washington's radioecological studies in the Marshall Islands, 1946-1977.

PubMed

Donaldson, L R; Seymour, A H; Nevissi, A E

1997-07-01

Since 1946, personnel from the School of Fisheries, University of Washington (Applied Fisheries Laboratory, 1943-1958; Laboratory of Radiation Biology, 1958-1967; and Laboratory of Radiation Ecology, since 1967), have studied the effects of nuclear detonations and the ensuing radioactivity on the marine and terrestrial environments throughout the Central Pacific. A collection of reports and publications about these activities plus a collection of several thousand samples from these periods are kept at the School of Fisheries. General findings from the surveys show that (1) fission products were prevalent in organisms of the terrestrial environment whereas activation products were prevalent in marine organisms; (2) the best biological indicators of fallout radionuclides by environments were (a) terrestrial-coconuts, land crabs; (b) reef-algae, invertebrates; and (c) marine-plankton, fish. Studies of plutonium and americium in Bikini Atoll showed that during 1971-1977 the highest concentrations of 241Am, 2.85 Bq g(-1) (77 pCi g(-1)) and 239,240Pu, 4.44 Bq g(-1) (120 pCi g(-1)), in surface sediments were found in the northwest part of the lagoon. The concentrations in the bomb craters were substantially lower than these values. Concentrations of soluble and particulate plutonium and americium in surface and deep water samples showed distributions similar to the sediment samples. That is, the highest concentration of these radionuclides in the water column were at locations with highest sediment concentration. Continuous circulation of water in the lagoon and exchange of water with open ocean resulted in removal of 111 G Bq y(-1) (3 Ci y(-1)) 241Am and 222 G Bq y(-1) (6 Ci y(-1)) 239,240Pu into the North Equatorial Current. A summary of the surveys, findings, and the historical role of the Laboratory in radioecological studies of the Marshall Islands are presented.

United States Transuranium and Uranium Registries. Annual Report, October 1, 1993--September 30, 1994

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kathren, R.L.; Harwick, L.A.

1995-08-01

This report summarizes the salient activities and progress of the United States Transuranium. and Uranium Registries for the period October 1, 1993 through September 30, 1994, along with details of specific programs areas including the National Human Radiobiology Tissue Repository (NHRTR) and tissue radiochemistry analysis project. Responsibility for tissue radioanalysis was transferred from Los Alamos National Laboratory to Washington State University in February 1994. The University of Washington was selected as the Quality Assurance/Quality Control laboratory and a three way intercomparison with them and LANL has been initiated. The results of the initial alpha spectrometry intercomparison showed excellent agreement amongmore » the laboratories and are documented in full in the Appendices to the report. The NHRTR serves as the initial point of receipt for samples received from participants in the USTUR program. Samples are weighed, divided, and reweighed, and a portion retained by the NHRTR as backup or for use in other studies. Tissue specimens retained in the NHRTR are maintained frozen at -70 C and include not only those from USTUR registrants but also those from the radium dial painter and thorium worker studies formerly conducted by Argonne National Laboratory. In addition, there are fixed tissues and a large collection of histopathology slides from all the studies, plus about 20,000 individual solutions derived from donated tissues. These tissues and tissue related materials are made available to other investigators for legitimate research purposes. Ratios of the concentration of actinides in various tissues have been used to evaluate the biokinetics, and retention half times of plutonium and americium. Retention half times for plutonium in various soft tissues range from 10-20 y except for the testes for which a retention half time of 58 y was observed. For americium, the retention half time in various soft tissues studied was 2.2-3.5 y.« less

Concentrations of plutonium and americium in plankton from the western Mediterranean Sea.

PubMed

Sanchez-Cabeza, Joan-Albert; Merino, Juan; Masqué, Pere; Mitchell, Peter I; Vintró, L León; Schell, William R; Cross, Lluïsa; Calbet, Albert

2003-07-20

Understanding the transfer of radionuclides through the food chain leading to man and in particular, the uptake of transuranic nuclides by plankton, is basic to assess the potential radiological risk of the consumption of marine products by man. The main sources of transuranic elements in the Mediterranean Sea in the past were global fallout and the Palomares accident, although at present smaller amounts are released from nuclear establishments in the northwestern region. Plankton from the western Mediterranean Sea was collected and analyzed for plutonium and americium in order to study their biological uptake. The microplankton fractions accounted for approximately 50% of the total plutonium contents in particulate form. At Garrucha (Palomares area), microplankton showed much higher 239,240 Pu activity, indicating the contamination with plutonium from the bottom sediments. Concentration factors were within the range of the values recommended by the International Atomic Energy Agency. Continental shelf mesoplankton was observed to efficiently concentrate transuranics. In open seawaters, concentrations were much lower. We speculate that sediments might play a role in the transfer of transuranics to mesoplankton in coastal waters, although we cannot discard that the difference in species composition may also play a role. In Palomares, both 239,240 Pu and 241Am showed activities five times higher than the mean values observed in continental shelf mesoplankton. As the plutonium isotopic ratios in the contaminated sample were similar to those found in material related to the accident, the contamination was attributed to bomb debris from the Palomares accident. Concentration factors in mesoplankton were also in relatively good agreement with the ranges recommended by IAEA. In the Palomares station the highest concentration factor was observed in the sample that showed predominance of the dynoflagellate Ceratium spp. Mean values of the enrichment factors showed, on average, discrimination rather than enrichment in the primary producer trophic chain.

241Am (n,gamma) isomer ratio measurement

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bond, Evelyn M; Vieira, David J; Moody, Walter A

The objective of this project is to improve the accuracy of the {sup 242}Cm/{sup 241}Am radiochemistry ratio. We have performed an activation experiment to measure the {sup 241}Am(n,{gamma}) cross section leading to either the ground state of {sup 242g}Am (t{sub 1/2} = 16 hr) which decays to {sup 242}Cm (t{sub 1/2} = 163 d) or the long-lived isomer {sup 242m}Am (t{sub 1/2} = 141 yr). This experiment will develop a new set of americium cross section evaluations that can be used with a measured {sup 242}Cm/{sup 241}Am radiochemical measurement for nuclear forensic purposes. This measurement is necessary to interpret themore » {sup 242}Cm/{sup 241}Am ratio because a good measurement of this neutron capture isomer ratio for {sup 241}Am does not exist. The targets were prepared in 2007 from {sup 241}Am purified from LANL stocks. Gold was added to the purified {sup 241}Am as an internal neutron fluence monitor. These targets were placed into a holder, packaged, and shipped to Forschungszentrum Karlsruhe, where they were irradiated at their Van de Graff facility in February 2008. One target was irradiated with {approx}25 keV quasimonoenergetic neutrons produced by the {sup 7}Li(p,n) reaction for 3 days and a second target was also irradiated for 3 days with {approx}500 keV neutrons. Because it will be necessary to separate the {sup 242}Cm from the {sup 241}Am in order to measure the amount of {sup 242}Cm by alpha spectrometry, research into methods for americium/curium separations were conducted concurrently. We found that anion exchange chromatography in methanol/nitric acid solutions produced good separations that could be completed in one day resulting in a sample with no residue. The samples were returned from Germany in July 2009 and were counted by gamma spectrometry. Chemical separations have commenced on the blank sample. Each sample will be spiked with {sup 244}Cm, dissolved and digested in nitric acid solutions. One third of each sample will be processed at a time. First, the gold will be removed by anion exchange chromatography. Then the {sup 242}Cm will be separated from the {sup 241}Am using the methanol/nitric acid anion exchange method. When a sufficient separation has been achieved, a deposit will be prepared and the {sup 242}Cm will be counted by alpha spectrometry. The purified {sup 241}Am fraction containing the long lived {sup 242m}Am will be allowed to decay into {sup 242}Cm for a period of {approx}6 months. After this time, the americium/curium separations will be repeated and the {sup 242}Cm that has grown in will be counted by alpha spectrometry. At the conclusion of the experiment, we will have cross section measurements for {sup 241}Am (n,{gamma}) {sup 242g}Am and {sup 241}Am (n,V) {sup 242m}Am at two energies.« less

Preparation of alpha-emitting nuclides by electrodeposition

NASA Astrophysics Data System (ADS)

Lee, M. H.; Lee, C. W.

2000-06-01

A method is described for electrodepositing the alpha-emitting nuclides. To determine the optimum conditions for plating plutonium, the effects of electrolyte concentration, chelating reagent, current, pH of electrolyte and the time of plating on the electrodeposition were investigated on the base of the ammonium oxalate-ammonium sulfate electrolyte containing diethyl triamino pentaacetic acid. An optimized electrodeposition procedure for the determination of plutonium was validated by application to environmental samples. The chemical yield of the optimized method of electrodeposition step in the environmental sample was a little higher than that of Talvitie's method. The developed electrodeposition procedure in this study was applied to determine the radionuclides such as thorium, uranium and americium that the electrodeposition yields were a little higher than those of the conventional method.

Evaluation of background concentrations of selected chemical and radiochemical constituents in water from the eastern Snake River Plain aquifer at and near the Idaho National Laboratory, Idaho

USGS Publications Warehouse

Bartholomay, Roy C.; L. Flint Hall,

2016-05-05

The upper limit of background concentrations for radiochemical constituents for eastern regional water was 5.43 ±0.574 pCi/L for tritium, 0.0002048 ±0.0000054 pCi/L for chlorine-36, 0.000000865 ±0.000000015 pCi/L for iodine-129, <0.0000054 pCi/L for technetium-99, 0 pCi/L for strontium-90, plutonium-238, plutonium-239, -240 (undivided), and americium-241, 1.32 ±0.77 pCi/L for uranium-234, 0.016 ±0.012 pCi/L for uranium-235, and 0.477 ±0.044 pCi/L for uranium-238.

Electronic and transformation properties of a metastable defect introduced in epitaxially grown boron-doped p-type Si by alpha particle irradiation

NASA Astrophysics Data System (ADS)

Mamor, M.; Auret, F. D.; Goodman, S. A.; Meyer, W. E.; Myburg, G.

1998-06-01

Titanium (Ti) Schottky barrier diodes on epitaxially grown boron-doped p-type Si films with a free carrier density of 6-8×1016cm-3 were irradiated with alpha particles at room temperature using an americium-241 (Am-241) radio nuclide. We report the electronic and transformation characteristics of an α-particle irradiation-induced defect Hα2 in epitaxially grown p-Si with metastable properties. The energy level and apparent capture cross section, as determined by deep-level transient spectroscopy, are Ev+0.43 eV and 1.4×10-15 cm2, respectively. This defect can be removed and re-introduced using a conventional bias-on/off cooling technique.

Preliminary study of neutron absorption by concrete with boron carbide addition

NASA Astrophysics Data System (ADS)

Abdullah, Yusof; Ariffin, Fatin Nabilah Tajul; Hamid, Roszilah; Yusof, Mohd Reusmaazran; Zali, Nurazila Mat; Ahmad, Megat Harun Al Rashid Megat; Yazid, Hafizal; Ahmad, Sahrim; Mohamed, Abdul Aziz

2014-02-01

Concrete has become a conventional material in construction of nuclear reactor due to its properties like safety and low cost. Boron carbide was added as additives in the concrete construction as it has a good neutron absorption property. The sample preparation for concrete was produced with different weight percent of boron carbide powder content. The neutron absorption rate of these samples was determined by using a fast neutron source of Americium-241/Be (Am-Be 241) and detection with a portable backscattering neutron detector. Concrete with 20 wt % of boron carbide shows the lowest count of neutron transmitted and this indicates the most neutrons have been absorbed by the concrete. Higher boron carbide content may affect the concrete strength and other properties.

Two new rodent models for actinide toxicity studies. [/sup 237/Pu, /sup 241/Am

DOE Office of Scientific and Technical Information (OSTI.GOV)

Taylor, G.N.; Jones, C.W.; Gardner, P.A.

1981-04-01

Two small rodent species, the grasshopper mouse (Onychomys leucogaster) and the deer mouse (Peromyscus maniculatus), have tenacious and high retention in the liver and skeleton of plutonium and americium following intraperitoneal injection of Pu and Am in citrate solution. Liver retention of Pu and Am in the grasshopper mouse is higher than liver retention in the deer mouse. Both of these rodents are relatively long-lived, breed well in captivity, and adapt suitably to laboratory conditions. It is suggested that these two species of mice, in which plutonium retention is high and prolonged in both the skeleton and liver, as itmore » is in man, may be useful animal models for actinide toxicity studies.« less

Probing the 5 f electrons in Am-I by hybrid density functional theory

NASA Astrophysics Data System (ADS)

Atta-Fynn, Raymond; Ray, Asok K.

2009-11-01

The ground states of the actinides and their compounds continue to be matters of considerable controversies. Experimentally, Americium-I (Am-I) is a non-magnetic dhcp metal whereas theoretically an anti-ferromagnetic ground state is predicted. We show that hybrid density functional theory, which admixes a fraction, λ, of exact Hartree-Fock (HF) exchange with approximate DFT exchange, can correctly reproduce the ground state properties of Am. In particular, for λ=0.40, we obtain a non-magnetic ground state with equilibrium atomic volume, bulk modulus, 5 f electron population, and the density of electronic states all in good agreement with experimental data. We argue that the exact HF exchange corrects the overestimation of the approximate DFT exchange interaction.

Utilization of Methacrylates and Polymer Matrices for the Synthesis of Ion Specific Resins

DOE Office of Scientific and Technical Information (OSTI.GOV)

Czerwinski, Kenneth

2013-10-29

Disposal, storage, and/or transmutation of actinides such as americium (Am) will require the development of specific separation schemes. Existing efforts focus on solvent extraction systems for achieving suitable separation of actinide from lanthanides. However, previous work has shown the feasibility of ion-imprinting polymer-based resins for use in ion-exchange-type separations with metal ion recognition. Phenolic-based resins have been shown to function well for Am-Eu separations, but these resins exhibited slow kinetics and difficulties in the imprinting process. This project addresses the need for new and innovative methods for the selective separation of actinides through novel ion-imprinted resins. The project team willmore » explore incorporation of metals into extended frameworks, including the possibility of 3D polymerized matrices that can serve as a solid-state template for specific resin preparation. For example, an anhydrous trivalent f-element chain can be formed directly from a metal carbonate, and methacrylic acid from water. From these simple coordination complexes, molecules of discrete size or shape can be formed via the utilization of coordinating ligands or by use of an anionic multi-ligand system incorporating methacrylate. Additionally, alkyl methyl methacrylates have been used successfully to create template nanospaces, which underscores their potential utility as 3D polymerized matrices. This evidence provides a unique route for the preparation of a specific metal ion template for the basis of ion-exchange separations. Such separations may prove to be excellent discriminators of metal ions, even between f-elements. Resins were prepared and evaluated for sorption behavior, column properties, and proton exchange capacity.« less

Development and application of anthropomorphic voxel phantom of the head for in vivo measurement.

PubMed

Vrba, T

2007-01-01

The in vivo measurement of the activity deposited in the skeleton is a very useful source of information on human internal contaminations with transuranic elements, e.g. americium 241, especially for long time periods after intake. Measurements are performed on the skull or the larger joints such as the knee or elbow. The paper deals with the construction of an anthropomorphic numerical phantom based on CT scans, its potential for calibration and the estimation of the uncertainties of the detection system. The density of bones, activity distribution and position of the detectors were changed in individual simulations in order to estimate their effects on the result of the measurement. The results from simulations with the numerical phantom were compared with the results of physical phantoms.

Pipe overpack container for trasuranic waste storage and shipment

DOEpatents

Geinitz, Richard R.; Thorp, Donald T.; Rivera, Michael A.

1999-01-01

A Pipe Overpack Container for transuranic waste storage and shipment. The system consists of a vented pipe component which is positioned in a vented, insulated 55 gallon steel drum. Both the vented pipe component and the insulated drum are capable of being secured to prevent the contents from leaving the vessel. The vented pipe component is constructed of 1/4 inch stainless steel to provide radiation shielding. Thus, allowing shipment having high Americium-241 content. Several Pipe Overpack Containers are then positioned in a type B, Nuclear Regulatory Commission (NRC) approved, container. In the current embodiment, a TRUPACT-II container was employed and a maximum of fourteen Pipe Overpack Containers were placed in the TRUPACT-II. The combination received NRC approval for the shipment and storage of transuranic waste.

Sorption--desorption studies on granite. I. Initial studies of strontium, technetium, cesium, barium, cerium, europium, uranium, plutonium, and americium

DOE Office of Scientific and Technical Information (OSTI.GOV)

Erdal, B.R.; Aguilar, R.D.; Bayhurst, B.P.

Distribution ratios were determined for sorption--desorption of radioactive tracers between the Climax Stock granite (quartz monzonite porphyry) obtained at Nevada Test Site and a water prepared to be resonably representative of the natural composition of water in equilibrium with the Climax Stock granite. The measurements were performed at 22 and 70{sup 0}C under atmospheric oxygen conditions. Elements given in order of increasing distribution coefficient at ambient temperature are: U(VI), Sr, Tc(VII), Ba, Ce(III), Cs, Eu(III), Pu, and Am. At 70{sup 0}C the order is: Tc(VII), Sr, Ce(III), Eu(III), Ba, Cs, Pu, and Am. The effects of surface area and mineralogymore » on sorption were also investigated.« less

Preliminary study of neutron absorption by concrete with boron carbide addition

DOE Office of Scientific and Technical Information (OSTI.GOV)

Abdullah, Yusof, E-mail: yusofabd@nuclearmalaysia.gov.my; Yusof, Mohd Reusmaazran; Zali, Nurazila Mat

2014-02-12

Concrete has become a conventional material in construction of nuclear reactor due to its properties like safety and low cost. Boron carbide was added as additives in the concrete construction as it has a good neutron absorption property. The sample preparation for concrete was produced with different weight percent of boron carbide powder content. The neutron absorption rate of these samples was determined by using a fast neutron source of Americium-241/Be (Am-Be 241) and detection with a portable backscattering neutron detector. Concrete with 20 wt % of boron carbide shows the lowest count of neutron transmitted and this indicates themore » most neutrons have been absorbed by the concrete. Higher boron carbide content may affect the concrete strength and other properties.« less

Assessment of the radionuclide composition of "hot particles" sampled in the Chernobyl nuclear power plant fourth reactor unit.

PubMed

Bondarkov, Mikhail D; Zheltonozhsky, Viktor A; Zheltonozhskaya, Maryna V; Kulich, Nadezhda V; Maksimenko, Andrey M; Farfán, Eduardo B; Jannik, G Timothy; Marra, James C

2011-10-01

Fuel-containing materials sampled from within the Chernobyl Nuclear Power Plant (ChNPP) Unit 4 Confinement Shelter were spectroscopically studied for gamma and alpha content. Isotopic ratios for cesium, europium, plutonium, americium, and curium were identified, and the fuel burn-up in these samples was determined. A systematic deviation in the burn-up values based on the cesium isotopes in comparison with other radionuclides was observed. The studies conducted were the first ever performed to demonstrate the presence of significant quantities of 242Cm and 243Cm. It was determined that there was a systematic underestimation of activities of transuranic radionuclides in fuel samples from inside of the ChNPP Confinement Shelter, starting from 241Am (and going higher) in comparison with the theoretical calculations.

Soft error evaluation and vulnerability analysis in Xilinx Zynq-7010 system-on chip

NASA Astrophysics Data System (ADS)

Du, Xuecheng; He, Chaohui; Liu, Shuhuan; Zhang, Yao; Li, Yonghong; Xiong, Ceng; Tan, Pengkang

2016-09-01

Radiation-induced soft errors are an increasingly important threat to the reliability of modern electronic systems. In order to evaluate system-on chip's reliability and soft error, the fault tree analysis method was used in this work. The system fault tree was constructed based on Xilinx Zynq-7010 All Programmable SoC. Moreover, the soft error rates of different components in Zynq-7010 SoC were tested by americium-241 alpha radiation source. Furthermore, some parameters that used to evaluate the system's reliability and safety were calculated using Isograph Reliability Workbench 11.0, such as failure rate, unavailability and mean time to failure (MTTF). According to fault tree analysis for system-on chip, the critical blocks and system reliability were evaluated through the qualitative and quantitative analysis.

Synthesis of dense yttrium-stabilised hafnia pellets for nuclear applications by spark plasma sintering

NASA Astrophysics Data System (ADS)

Tyrpekl, Vaclav; Holzhäuser, Michael; Hein, Herwin; Vigier, Jean-Francois; Somers, Joseph; Svora, Petr

2014-11-01

Dense yttrium-stabilised hafnia pellets (91.35 wt.% HfO2 and 8.65 wt.% Y2O3) were prepared by spark plasma sintering consolidation of micro-beads synthesised by the "external gelation" sol-gel technique. This technique allows a preparation of HfO2-Y2O3 beads with homogenous yttria-hafnia solid solution. A sintering time of 5 min at 1600 °C was sufficient to produce high density pellets (over 90% of the theoretical density) with significant reproducibility. The pellets have been machined in a lathe to the correct dimensions for use as neutron absorbers in an experimental test irradiation in the High Flux Reactor (HFR) in Petten, Holland, in order to investigate the safety of americium based nuclear fuels.

Measurement of actinides and strontium-90 in high activity waste

DOE Office of Scientific and Technical Information (OSTI.GOV)

Maxwell, S.L. III; Nelson, M.R.

1994-08-01

The reliable measurement of trace radionuclides in high activity waste is important to support waste processing activities at SRS (F and H Area Waste Tanks, Extended Sludge Processing (ESP) and In-Tank precipitation (ITP) processing). Separation techniques are needed to remove high levels of gamma activity and alpha/beta interferences prior to analytical measurement. Using new extraction chromatographic resins from EiChrom Industries, Inc., the SRS Central Laboratory has developed new high speed separation methods that enable measurement of neptunium, thorium, uranium, plutonium, americium and strontium-90 in high activity waste solutions. Small particle size resin and applied vacuum are used to reduce analysismore » times and enhance column performance. Extraction chromatographic resins are easy to use and eliminate the generation of contaminated liquid organic waste.« less

Electrolytic decontamination of conductive materials for hazardous waste management

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wedman, D.E.; Martinez, H.E.; Nelson, T.O.

1996-12-31

Electrolytic removal of plutonium and americium from stainless steel and uranium surfaces has been demonstrated. Preliminary experiments were performed on the electrochemically based decontamination of type 304L stainless steel in sodium nitrate solutions to better understand the metal removal effects of varying cur-rent density, pH, and nitrate concentration parameters. Material removal rates and changes in surface morphology under these varying conditions are reported. Experimental results indicate that an electropolishing step before contamination removes surface roughness, thereby simplifying later electrolytic decontamination. Sodium nitrate based electrolytic decontamination produced the most uniform stripping of material at low to intermediate pH and at sodiummore » nitrate concentrations of 200 g L{sup -1} and higher. Stirring was also observed to increase the uniformity of the stripping process.« less

Nevada applied ecology group publications

DOE Office of Scientific and Technical Information (OSTI.GOV)

Chilton, B.D.; Pfuderer, H.A.; Cox, T.L.

Since January 1972, the Nevada Applied Ecology Information Center (NAEIC), Information Research and Analysis Section, Health and Safety Research Division, Oak Ridge National Laboratory, has provided technical information support to the Nevada Applied Ecology Group (NAEG) relevant to the behavior of specific radionuclides, primarily plutonium and americium, in the environment, with special emphasis on pathways to man. This bibliography represents a summary of the biomedical and environmental studies conducted by the NAEG and its contractors. The bibliography focuses on research sponsored by the NAEG. Subject areas of the publications include cover studies of soil, vegetation, animals, microorganisms, resuspension, and meteorology.more » All references in this publication are stored in a computerized form that is readily available for searches upon request to NAEG and it contractors. 558 refs.« less

Impact of the deployment schedule of fast breeding reactors in the frame of French act for nuclear materials and radioactive waste management

DOE Office of Scientific and Technical Information (OSTI.GOV)

Le Mer, J.; Garzenne, C.; Lemasson, D.

In the frame of the French Act of June 28, 2006 on 'a sustainable management of nuclear materials and radioactive waste' EDF R and D assesses various research scenarios of transition between the actual French fleet and a Generation IV fleet with a closed fuel cycle where plutonium is multi-recycled. The basic scenarios simulate a deployment of 60 GWe of Sodium-cooled Fast Reactors (SFRs) in two steps: one third from 2040 to 2050 and the rest from 2080 to 2100 (scenarios 2040). These research scenarios assume that SFR technology will be ready for industrial deployment in 2040. One of themore » many sensitivity analyses that EDF, as a nuclear power plant operator, must evaluate is the impact of a delay of SFR technology in terms of uranium consumptions, plutonium needs and fuel cycle utilities gauging. The sensitivity scenarios use the same assumptions as scenarios 2040 but they simulate a different transition phase: SFRs are deployed in one step between 2080 and 2110 (scenarios 2080). As the French Act states to conduct research on minor actinides (MA) management, we studied different options for 2040 and 2080 scenarios: no MA transmutation, americium transmutation in heterogeneous mode based on americium Bearing Blankets (AmBB) in SFRs and all MA transmutation in heterogeneous mode based on MA Bearing Blankets (MABB). Moreover, we studied multiple parameters that could impact the deployment of these reactors (SFR load factor, increase of the use of MOX in Light Water Reactors, increase of the cooling time in spent nuclear fuel storage...). Each scenario has been computed with the EDF R and D fuel cycle simulation code TIRELIRE-STRATEGIE and optimized to meet various fuel cycle constraints such as using the reprocessing facility with long period of constant capacity, keeping the temporary stored mass of plutonium and MA under imposed limits, recycling older assemblies first... These research scenarios show that the transition from the current PWR fleet to an equivalent fleet of Generation IV SFR can follow different courses. The design of SFR-V2B that we used in our studies needs a high inventory of plutonium resulting in tension on this resource. Several options can be used in order to loosen this tension: our results lead to favour the use of axial breeding blanket in SFR. Load factor of upcoming reactors has to be regarded with attention as it has a high impact on plutonium resource for a given production of electricity. The deployment of SFRs beginning in 2080 instead of 2040 following the scenarios we described creates higher tensions on reprocessing capacity, separated plutonium storage and spent fuel storage. In the frame of the French Act, we studied minor actinides transmutation. The flux of MA in all fuel cycle plants is really high, which will lead to decay heat, a and neutron emission related problems. In terms of reduction of MA inventories, the deployment of MA transmutation cycle must not delay the installation of SFRs. The plutonium production in MABB and AmBB does not allow reducing the use of axial breeding blankets. The impact of MA or Am transmutation over the high level waste disposal is more important if the SFRs are deployed later. Transmutation option (americium or all MA) does not have a significant impact on the number of canister produced nor on its long-term thermal properties. (authors)« less

Improved sample utilization in thermal ionization mass spectrometry isotope ratio measurements: refined development of porous ion emitters for nuclear forensic applications

DOE Office of Scientific and Technical Information (OSTI.GOV)

Baruzzini, Matthew Louis

The precise and accurate determination of isotopic composition in nuclear forensic samples is vital for assessing origin, intended use and process history. Thermal ionization mass spectrometry (TIMS) is widely accepted as the gold standard for high performance isotopic measurements and has long served as the workhorse in the isotopic ratio determination of nuclear materials. Nuclear forensic and safeguard specialists have relied heavily on such methods for both routine and atypical e orts. Despite widespread use, TIMS methods for the assay of actinide systems continue to be hindered by poor ionization e ciency, often less than tenths of a percent; themore » majority of a sample is not measured. This represents a growing challenge in addressing nextgeneration nuclear detection needs by limiting the ability to analyze ultratrace quantities of high priority elements that could potentially provide critical nuclear forensic signatures. Porous ion emitter (PIE) thermal ion sources were developed in response to the growing need for new TIMS ion source strategies for improved ionization e ciency, PIEs have proven to be simple to implement, straightforward approach to boosting ion yield. This work serves to expand the use of PIE techniques for the analysis of trace quantities of plutonium and americium. PIEs exhibited superior plutonium and americium ion yields when compared to direct lament loading and the resin bead technique, one of the most e cient methods for actinide analysis, at similar mass loading levels. Initial attempts at altering PIE composition for the analysis of plutonium proved to enhance sample utilization even further. Preliminary investigations of the instrumental fractionation behavior of plutonium and uranium analyzed via PIE methods were conducted. Data collected during these initial trial indicate that PIEs fractionate in a consistent, reproducible manner; a necessity for high precision isotope ratio measurements. Ultimately, PIEs methods were applied for the age determination of various uranium isotopic standards. PIEs did not exhibit signi cant advantages for the determination of model ages when compared to traditional laments; however, this trial was able to provide valuable insight for guiding future investigations.« less

Aerial Measuring System Sensor Modeling

DOE Office of Scientific and Technical Information (OSTI.GOV)

R. S. Detwiler

2002-04-01

This project deals with the modeling the Aerial Measuring System (AMS) fixed-wing and rotary-wing sensor systems, which are critical U.S. Department of Energy's National Nuclear Security Administration (NNSA) Consequence Management assets. The fixed-wing system is critical in detecting lost or stolen radiography or medical sources, or mixed fission products as from a commercial power plant release at high flying altitudes. The helicopter is typically used at lower altitudes to determine ground contamination, such as in measuring americium from a plutonium ground dispersal during a cleanup. Since the sensitivity of these instruments as a function of altitude is crucial in estimatingmore » detection limits of various ground contaminations and necessary count times, a characterization of their sensitivity as a function of altitude and energy is needed. Experimental data at altitude as well as laboratory benchmarks is important to insure that the strong effects of air attenuation are modeled correctly. The modeling presented here is the first attempt at such a characterization of the equipment for flying altitudes. The sodium iodide (NaI) sensors utilized with these systems were characterized using the Monte Carlo N-Particle code (MCNP) developed at Los Alamos National Laboratory. For the fixed wing system, calculations modeled the spectral response for the 3-element NaI detector pod and High-Purity Germanium (HPGe) detector, in the relevant energy range of 50 keV to 3 MeV. NaI detector responses were simulated for both point and distributed surface sources as a function of gamma energy and flying altitude. For point sources, photopeak efficiencies were calculated for a zero radial distance and an offset equal to the altitude. For distributed sources approximating an infinite plane, gross count efficiencies were calculated and normalized to a uniform surface deposition of 1 {micro}Ci/m{sup 2}. The helicopter calculations modeled the transport of americium-241 ({sup 241}Am) as this is the ''marker'' isotope utilized by the system for Pu detection. The helicopter sensor array consists of 2 six-element NaI detector pods, and the NaI pod detector response was simulated for a distributed surface source of {sup 241}Am as a function of altitude.« less

An ab initio study of the adsorption and dissociation of molecular oxygen on the (0 0 0 1) surface of double hexagonal close-packed americium

NASA Astrophysics Data System (ADS)

Dholabhai, Pratik P.; Atta-Fynn, Raymond; Ray, Asok K.

2008-12-01

In our continuing attempts to understand theoretically various surface properties such as corrosion and potential catalytic activity of actinide surfaces in the presence of environmental gases, we report here the first ab initio study of molecular adsorption on the double hexagonal close-packed (dhcp) americium (Am) (0 0 0 1) surface. Specifically, molecular oxygen adsorption on the (0 0 0 1) surface of dhcp Am has been studied in detail within the framework of density functional theory using a full-potential all-electron linearized augmented plane wave plus local orbitals (FP-LAPW+lo) method. Dissociative adsorption is found to be energetically more favorable compared to molecular adsorption. Chemisorption energies were optimized with respect to the distance of adsorbates from the surface for three approach positions at three adsorption sites, namely t1 (one-fold top), b2 (two-fold bridge), and h3 (three-fold hollow) sites. Chemisorption energies were computed at the scalar-relativistic-no-spin-orbit-coupling (SR-NSOC) and at the fully relativistic-with-spin-orbit-coupling (FR-SOC) levels of theory. The most stable configuration corresponds to a horizontal approach molecular dissociation with the oxygen atoms occupying neighboring h3 sites, with chemisorption energies at the NSOC and SOC theoretical levels being 9.395 and 9.886 eV, respectively. The corresponding distances of the oxygen molecule from the surface and oxygen-oxygen distance were found to be 0.953 and 3.731 Å, respectively. Overall our calculations indicate that chemisorption energies in cases with SOC are slightly more stable than those with NSOC in the 0.089-0.493 eV range. The work functions and net magnetic moments, respectively, increased and decreased in all cases compared to corresponding quantities of the bare dhcp-Am (0 0 0 1) surface. Adsorbate-substrate interactions have been analyzed in detail using partial charges inside muffin-tin spheres, difference charge density distributions, and the local density of states. The effects, if any, of chemisorption on Am5f electron localization-delocalization characteristics in the vicinity of the Fermi level are also discussed.

Extraction of water and speciation of trivalent lanthanides and americium in organophosphorus extractants

DOE PAGES

Gullekson, Brian J.; Breshears, Andrew T.; Brown, M. Alex; ...

2016-11-29

Complexes of the trivalent lanthanides and Am with di-2-ethylhexylphosphoric acid (HDEHP) dissolved in an aliphatic diluent were probed with UV–vis, X-ray absorption fine structure, and time-resolved fluorescence spectroscopy while the water concentration was determined by Karl Fischer titrations. In particular, our work focuses on the Nd-hypersensitive UV–vis absorbance region to identify the cause of changing absorbance values at 570 and 583 nm in relation to the pseudooctahedral Nd environment when coordinated with three HDEHP dimers. In contrast to recently reported interpretations, we establish that while impurities have an effect on this electronic transition band, a high water content can causemore » distortion of the pseudooctahedral symmetry of the six-coordinate Nd, resembling the reported spectra of the seven-coordinate Nd compounds. Extended X-ray absorption fine structure analysis of the Nd in high-concentration HDEHP solutions also points to an increase in the coordination number from 6 to 7. The spectral behavior of other lanthanides (Pr, Ho, Sm, and Er) and Am III as a function of the HDEHP concentration suggests that water coordination with the metal likely depends on the metal’s effective charge. Fluorescence data using lifetime studies and excitation and emission spectra support the inclusion of water in the Eu coordination sphere. Further, the role of the effective charge was confirmed by a comparison of the Gibbs free energies of six- and seven-coordinate La-HDEHP–H 2O and Lu-HDEHP–H 2O complexes using density functional theory. In contrast, HEH[EHP], the phosphonic acid analogue of HDEHP, exhibits a smaller capacity for water, and the electronic absorption spectra of Nd or Am appear to be unchanged, although the Pr spectra show a noticeable change in intensity as a function of the water content. As a result, electronic absorption extinction coefficients of Am III, Nd III, Pr III, Sm III, Er III, and Ho III as a function of the HDEHP concentration are reported for the first time.« less

Extraction of water and speciation of trivalent lanthanides and americium in organophosphorus extractants

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gullekson, Brian J.; Breshears, Andrew T.; Brown, M. Alex

Complexes of the trivalent lanthanides and Am with di-2-ethylhexylphosphoric acid (HDEHP) dissolved in an aliphatic diluent were probed with UV–vis, X-ray absorption fine structure, and time-resolved fluorescence spectroscopy while the water concentration was determined by Karl Fischer titrations. In particular, our work focuses on the Nd-hypersensitive UV–vis absorbance region to identify the cause of changing absorbance values at 570 and 583 nm in relation to the pseudooctahedral Nd environment when coordinated with three HDEHP dimers. In contrast to recently reported interpretations, we establish that while impurities have an effect on this electronic transition band, a high water content can causemore » distortion of the pseudooctahedral symmetry of the six-coordinate Nd, resembling the reported spectra of the seven-coordinate Nd compounds. Extended X-ray absorption fine structure analysis of the Nd in high-concentration HDEHP solutions also points to an increase in the coordination number from 6 to 7. The spectral behavior of other lanthanides (Pr, Ho, Sm, and Er) and Am III as a function of the HDEHP concentration suggests that water coordination with the metal likely depends on the metal’s effective charge. Fluorescence data using lifetime studies and excitation and emission spectra support the inclusion of water in the Eu coordination sphere. Further, the role of the effective charge was confirmed by a comparison of the Gibbs free energies of six- and seven-coordinate La-HDEHP–H 2O and Lu-HDEHP–H 2O complexes using density functional theory. In contrast, HEH[EHP], the phosphonic acid analogue of HDEHP, exhibits a smaller capacity for water, and the electronic absorption spectra of Nd or Am appear to be unchanged, although the Pr spectra show a noticeable change in intensity as a function of the water content. As a result, electronic absorption extinction coefficients of Am III, Nd III, Pr III, Sm III, Er III, and Ho III as a function of the HDEHP concentration are reported for the first time.« less

Effect of solvent on in vitro dissolution: Summary of results for uranium, americium, and cobalt aerosols

DOE Office of Scientific and Technical Information (OSTI.GOV)

Guilmette, R.A.; Hoover, M.D.

1995-12-01

The revised 10 CFR Part 20 has adopted the ICRP Publication 30 method for calculating the committed effective dose equivalent from intakes of radionuclides. This dosimetry scheme requires knowledge or assumptions about the chemical form of the radionuclide, its particle size, and its known or assumed solubility. The solubility is classified as being either D (relatively soluble), W, or Y (relatively insoluble), depending on whether the material dissolves over periods of days, weeks, or years. Although Nuclear Regulatory Commission licensees may wish to take advantage of material-specific knowledge in order to adjust annual limits on intake and derived air concentrations,more » relatively few radioactive materials to which workers and the general population may be exposed have been adequately characterized either in terms of physicochemical form or solubility. Experimental measurement of solubility using some type of in vitro dissolution measurement system is therefore needed. However, there is currently no clear consensus regarding the appropriate design of in vitro dissolution systems, particularly when considering the range of different radionuclides to be studied, and the complexity of the biological mechanisms involved in the retention and clearance of inhaled deposited radioactive particles. The purpose of this study was to evaluate the effect of the several solvents on the dissolution of four test aerosols ({sup 57}Co{sub 3}O{sub 4}, {sup 241}AmO{sub 2}, ammonium diuranate [ADU], and U{sub 3}O{sub 8}) selected to encompass a variety of chemical and biochemical properties in vivo. The results of this study provide some guidance on the usefulness of in vitro dissolution tests for estimating the solubility of unknown radionuclide particles within the context of a simple model such as the class D, W, and Y formulation of ICRP 30.« less

Migration of conservative and sorbing radionuclides in heterogeneous fractured rock aquifers at the Nevada Test Site

NASA Astrophysics Data System (ADS)

Boryta, J. R.; Wolfsberg, A. V.

2003-12-01

The Nevada Test Site (NTS) is the United States continental nuclear weapons testing site. The larger underground tests, including BENHAM and TYBO, were conducted at Pahute Mesa. The BENHAM test, conducted in 1968, was detonated 1.4 km below the surface and the TYBO test, conducted in 1975, was detonated at a depth of 765 m. Between 1996 and 1998, several radionuclides were discovered in trace concentrations in a monitoring well complex 273 m from TYBO and 1300 m from BENHAM. Previous studies associated with these measurements have focused primarily on a) plutonium discovered in the observation wells, which was identified through isotopic finger printing as originating at BENHAM, b) colloid-facilitated plutonium transport processes, and c) vertical convection in subsurface nuclear test collapse chimneys. In addition to plutonium, several other non-, weakly-, and strongly-sorbing radionuclides were discovered in trace concentrations in the observation wells, including tritium, carbon-14, chlorine-36, iodine-129, technetium-99, neptunium-237, strontium-90, cesium-137, americium-241, and europium-152,154,155. The range in retardation processes affecting these different radionuclides provides additional information for assessing groundwater solute transport model formulations. For all radionuclides, simulation results are most sensitive to the fracture porosity and fracture aperture. Additionally, for weakly sorbing Np, simulation results are highly sensitive to the matrix sorption coefficient. For strongly sorbing species, migration in the absence of colloids can only be simulated if fracture apertures are set very large, reducing the amount of diffusion that can occur. For these species, colloid-facilitated transport appears to be a more likely explanation for the measurements. This is corroborated with colloid-transport model simulations.

ASSESSMENT OF THE RADIONUCLIDE COMPOSITION OF "HOT PARTICLES" SAMPLED IN THE CHERNOBYL NUCLEAR POWER PLANT FOURTH REACTOR UNIT

DOE Office of Scientific and Technical Information (OSTI.GOV)

Farfan, E.; Jannik, T.; Marra, J.

2011-10-01

Fuel-containing materials sampled from within the Chernobyl Nuclear Power Plant (ChNPP) 4th Reactor Unit Confinement Shelter were spectroscopically studied for gamma and alpha content. Isotopic ratios for cesium, europium, plutonium, americium, and curium were identified and the fuel burnup in these samples was determined. A systematic deviation in the burnup values based on the cesium isotopes, in comparison with other radionuclides, was observed. The conducted studies were the first ever performed to demonstrate the presence of significant quantities of {sup 242}Cm and {sup 243}Cm. It was determined that there was a systematic underestimation of activities of transuranic radionuclides in fuelmore » samples from inside of the ChNPP Confinement Shelter, starting from {sup 241}Am (and going higher), in comparison with the theoretical calculations.« less

Decorporation of inhaled americium-241 dioxide and nitrate from hamsters using ZnDTPA and Puchel.

PubMed

Stradling, G N; Stather, J W; Sumner, S A; Moody, J C; Strong, J C

1984-06-01

Accidental intakes of 241AmO2 and 241Am(NO3)3 can be treated with some success by inhalation of ZnDTPA . The main advantage of this method of treatment is that it can be self-administered very soon after an accidental intake, and it is effective for reducing the lung content of Am at doses about 10 times less than those usually used intravenously. Otherwise the efficacy of injected ZnDTPA is superior since in addition to removing 241Am from the lungs it can deplete appreciably the systemic deposit of the nuclide. There appears to be no advantage in using the lipophilic form of DTPA code-named Puchel , since following the inhalation or injection of the compound decorporation is not significantly increased relative to ZnDTPA .

Pipe overpack container for transuranic waste storage and shipment

DOE Office of Scientific and Technical Information (OSTI.GOV)

Geinitz, R.R.; Thorp, D.T.; Rivera, M.A.

1999-12-07

A Pipe Overpack Container is described for transuranic waste storage and shipment. The system consists of a vented pipe component which is positioned in a vented, insulated 55 gallon steel drum. Both the vented pipe component and the insulated drum are capable of being secured to prevent the contents from leaving the vessel. The vented pipe component is constructed of 1/4 inch stainless steel to provide radiation shielding, thus allowing shipment having high Americium-241 content. Several Pipe Overpack Containers are then positioned in a type B, Nuclear Regulatory Commission (NRC) approved, container. In the current embodiment, a TRUPACT-II container wasmore » employed and a maximum of fourteen Pipe Overpack Containers were placed in the TRUPACT-II. The combination received NRC approval for the shipment and storage of transuranic waste.« less

Fabrication of (U,Am)O2 pellet with controlled porosity from oxide microspheres

NASA Astrophysics Data System (ADS)

Ramond, Laure; Coste, Philippe; Picart, Sébastien; Gauthé, Aurélie; Bataillea, Marc

2017-08-01

U1-xAmxO2±δ mixed-oxides are considered as promising compounds for americium heterogeneous transmutation in Sodium Fast Neutron Reactor. Porous microstructure is envisaged in order to facilitate helium and fission gas release and to reduce pellet swelling during irradiation and under self-irradiation. In this study, the porosity is created by reducing (U,Am)3O8 microspheres into (U,Am)O2 during the sintering. This reduction is accompanied by a decrease of the lattice volume that leads to the creation of open porosity. Finally, an (U0.90Am0.10)O2 porous ceramic pellet (D∼89% of the theoretical density TD) with controlled porosity (≥8% open porosity) was obtained from mixed-oxide microspheres obtained by the Weak Acid Resin (WAR) process.

Continuous transport of Pacific-derived anthropogenic radionuclides towards the Indian Ocean

PubMed Central

Pittauer, Daniela; Tims, Stephen G.; Froehlich, Michaela B.; Fifield, L. Keith; Wallner, Anton; McNeil, Steven D.; Fischer, Helmut W.

2017-01-01

Unusually high concentrations of americium and plutonium have been observed in a sediment core collected from the eastern Lombok Basin between Sumba and Sumbawa Islands in the Indonesian Archipelago. Gamma spectrometry and accelerator mass spectrometry data together with radiometric dating of the core provide a high-resolution record of ongoing deposition of anthropogenic radionuclides. A plutonium signature characteristic of the Pacific Proving Grounds (PPG) dominates in the first two decades after the start of the high yield atmospheric tests in 1950’s. Approximately 40–70% of plutonium at this site in the post 1970 period originates from the PPG. This sediment record of transuranic isotopes deposition over the last 55 years provides evidence for the continuous long-distance transport of particle-reactive radionuclides from the Pacific Ocean towards the Indian Ocean. PMID:28304374

Distributions of Pu, Am and Cs in margin sediments from the western Mediterranean (Spanish coast).

PubMed

Gascó, C; Antón, M P; Pozuelo, M; Meral, J; González, A M; Papucci, C; Delfanti, R

2002-01-01

Continental margins are important areas to be considered when studying the distributions and depositions of pollutants, both conventional and radioactive. Coastal sediments accumulate most of those contaminants which can be introduced following atmospheric and/or fluvial pathways. Moreover, their residence times within the water column are usually shortened due to their affinity to associate with the downward falling particulate matter, more abundant at shallower depths. In this paper the distribution profiles and inventories of plutonium, americium and cesium are detailed, providing useful information about recent sedimentation phenomena such as sediment mixing, slumping processes and bioturbation. Unsupported 210Pb data are used as reliable indicators of enhanced/reduced deposition events. Also, the calculated inventories have enabled the estimation of the radiological contribution of the Spanish Mediterranean margin to the total radioactivity deposited onto the Mediterranean sea floor.

Monte Carlo simulation of the operational quantities at the realistic mixed neutron-photon radiation fields CANEL and SIGMA.

PubMed

Lacoste, V; Gressier, V

2007-01-01

The Institute for Radiological Protection and Nuclear Safety owns two facilities producing realistic mixed neutron-photon radiation fields, CANEL, an accelerator driven moderator modular device, and SIGMA, a graphite moderated americium-beryllium assembly. These fields are representative of some of those encountered at nuclear workplaces, and the corresponding facilities are designed and used for calibration of various instruments, such as survey meters, personal dosimeters or spectrometric devices. In the framework of the European project EVIDOS, irradiations of personal dosimeters were performed at CANEL and SIGMA. Monte Carlo calculations were performed to estimate the reference values of the personal dose equivalent at both facilities. The Hp(10) values were calculated for three different angular positions, 0 degrees, 45 degrees and 75 degrees, of an ICRU phantom located at the position of irradiation.

AmO 2 Analysis for Analytical Method Testing and Assessment: Analysis Support for AmO 2 Production

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kuhn, Kevin John; Bland, Galey Jean; Fulwyler, James Brent

Americium oxide samples will be measured for various analytes to support AmO 2 production. The key analytes that are currently requested by the Am production customer at LANL include total Am content, Am isotopics, Pu assay, Pu isotopics, and trace element content including 237Np content. Multiple analytical methods will be utilized depending on the sensitivity, accuracy and precision needs of the Am matrix. Traceability to the National Institute of Standards and Technology (NIST) will be achieved, where applicable, by running NIST traceable quality control materials. This given that there are no suitable AmO 2 reference materials currently available for requestedmore » analytes. The primary objective is to demonstrate the suitability of actinide analytical chemistry methods to support AmO 2 production operations.« less

Transuranic biokinetic parameters for marine invertebrates--a review.

PubMed

Ryan, T P

2002-04-01

A catalogue of biokinetic parameters for the transuranic elements plutonium, americium, curium, neptunium, and californium in marine invertebrates is presented. The parameters considered are: the seawater-animal concentration factor (CF); the sediment-animal concentration ratio (CR); transuranic assimilation efficiency; transuranic tissue distribution and transuranic elimination rates. With respect to the seawater-animal CF, authors differ considerably on how they define this parameter and a seven-point reporting system is suggested. Transuranic uptake from sediment by animals is characterised by low CRs. The assimilation efficiencies of transuranic elements in marine invertebrates are high compared to vertebrates and mammals in general and the distribution of transuranics within the body tissue of an animal is dependent on the uptake path. The elimination of transuranics from most species examined conformed to a standard biphasic exponential model though some examples with three elimination phases were identified.

Separation of americium from europium using 3,3'-dimethoxy-phenyl-bis-1,2,4-triazinyl-2,6-pyridine

DOE PAGES

Hill, Talon G.; Chin, Ai Lin; Tai, Serene; ...

2017-03-22

Development of liquid-liquid separation processes for the effective removal of the minor actinide Am(III) from used nuclear fuel using ligand-based strategies continues to be an area of significant research focus. The current investigation demonstrates the efficacy of a nitrogen-based bis-triazinyl pyridine (BTP) derivative to selectively extract Am(III) from nitric acid solutions containing light lanthanides. The performance of 3,3’-dimethoxy-phenyl-bis-1,2,4-triazinyl-2,6- pyridine (MOB-BTP) was compared to that of a camphor substituted BTP (CA-BTP). The results of this investigation demonstrate the novel 3,3’-methoxy-BTP extractant dissolved in a polar diluent was a more efficient extractant for Am(III) at a lower concentration than CA-BTP under comparablemore » conditions.« less

Separation of americium from europium using 3,3'-dimethoxy-phenyl-bis-1,2,4-triazinyl-2,6-pyridine

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hill, Talon G.; Chin, Ai Lin; Tai, Serene

Development of liquid-liquid separation processes for the effective removal of the minor actinide Am(III) from used nuclear fuel using ligand-based strategies continues to be an area of significant research focus. The current investigation demonstrates the efficacy of a nitrogen-based bis-triazinyl pyridine (BTP) derivative to selectively extract Am(III) from nitric acid solutions containing light lanthanides. The performance of 3,3’-dimethoxy-phenyl-bis-1,2,4-triazinyl-2,6- pyridine (MOB-BTP) was compared to that of a camphor substituted BTP (CA-BTP). The results of this investigation demonstrate the novel 3,3’-methoxy-BTP extractant dissolved in a polar diluent was a more efficient extractant for Am(III) at a lower concentration than CA-BTP under comparablemore » conditions.« less

Contributions of Various Radiological Sources to Background in a Suburban Environment

DOE PAGES

Milvenan, Richard D.; Hayes, Robert B.

2016-11-01

This work is a brief overview and comparison of dose rates stemming from both indoor and outdoor natural background radiation and household objects within a suburban environment in North Carolina. Combined gamma and beta dose rates were taken from indoor objects that ranged from the potassium in fruit to the americium in smoke detectors. For outdoor measurements, various height and time data samples were collected to show fluctuations in dose rate due to temperature inversion and geometric attenuation. Although each sample tested proved to have a statistically significant increase over background using Students t-test, no sample proved to be moremore » than a minor increase in natural radiation dose. Furthermore, the relative contributions from natural radioactivity such as potassium in foods and common household items are shown to be easily distinguished from background using standard handheld instrumentation when applied in a systematic, methodological manner.« less

Metallic Fuel Casting Development and Parameter Optimization Simulations

DOE Office of Scientific and Technical Information (OSTI.GOV)

R.S. Fielding; J. Crapps; C. Unal

One of the advantages of metallic fuel is the abilility to cast the fuel slugs to near net shape with little additional processing. However, the high aspect ratio of the fuel is not ideal for casting. EBR-II fuel was cast using counter gravity injection casting (CGIC) but, concerns have been raised concerning the feasibility of this process for americium bearing alloys. The Fuel Cycle Research and Development program has begun developing gravity casting techniques suitable for fuel production. Compared to CGIC gravity casting does not require a large heel that then is recycled, does not require application of a vacuummore » during melting, and is conducive to re-usable molds. Development has included fabrication of two separate benchscale, approximately 300 grams, systems. To shorten development time computer simulations have been used to ensure mold and crucible designs are feasible and to identify which fluid properties most affect casting behavior and therefore require more characterization.« less

Selected quality assurance data for water samples collected by the US Geological Survey, Idaho National Engineering Laboratory, Idaho, 1980 to 1988

USGS Publications Warehouse

Wegner, S.J.

1989-01-01

Multiple water samples from 115 wells and 3 surface water sites were collected between 1980 and 1988 for the ongoing quality assurance program at the Idaho National Engineering Laboratory. The reported results from the six laboratories involved were analyzed for agreement using descriptive statistics. The constituents and properties included: tritium, plutonium-238, plutonium-239, -240 (undivided), strontium-90, americium-241, cesium-137, total dissolved chromium, selected dissolved trace metals, sodium, chloride, nitrate, selected purgeable organic compounds, and specific conductance. Agreement could not be calculated for purgeable organic compounds, trace metals, some nitrates and blank sample analyses because analytical uncertainties were not consistently reported. However, differences between results for most of these data were calculated. The blank samples were not analyzed for differences. The laboratory results analyzed using descriptive statistics showed a median agreement between all useable data pairs of 95%. (USGS)

Variations in AmLi source spectra and their estimation utilizing the 5 Ring Multiplicity Counter

DOE PAGES

Weinmann-Smith, Robert; Beddingfield, David H.; Enqvist, Andreas; ...

2017-02-28

Active-mode assay systems are widely used for the safeguards of uranium items to verify compliance with the Non-Proliferation Treaty. Systems such as the Active-Well Coincidence Counter (AWCC) and the Uranium Neutron Coincidence Collar (UNCL) use americium-lithium (AmLi) neutron sources to induce fissions which are measured to determine the sample mass. These systems have historically relied on calibrations derived from well-defined standards. Recently, restricted access to standards or more difficult measurements have resulted in a reliance on modeling and simulation for the calibration of systems, which introduces potential simulation biases. Furthermore, the AmLi source energy spectra commonly used in the safeguardsmore » community do not accurately represent measurement results and the spectrum uncertainty can represent a large contribution to the total modeling uncertainty in active-mode systems.« less

Multiscale structural characterizations of mixed U(iv)-An(iii) oxalates (An(iii) = Pu or Am) combining XAS and XRD measurements.

PubMed

Arab-Chapelet, B; Martin, P M; Costenoble, S; Delahaye, T; Scheinost, A C; Grandjean, S; Abraham, F

2016-04-28

Mixed actinide(III,IV) oxalates of the general formula M2.2UAn(C2O4)5·nH2O (An = Pu or Am and M = H3O(+) and N2H5(+)) have been quantitatively precipitated by oxalic precipitation in nitric acid medium (yield >99%). Thorough multiscale structural characterization using XRD and XAS measurements confirmed the existence of mixed actinide oxalate solid solutions. The XANES analysis confirmed that the oxidation states of the metallic cations, tetravalent for uranium and trivalent for plutonium and americium, are maintained during the precipitation step. EXAFS measurements show that the local environments around U(+IV), Pu(+III) and Am(+III) are comparable, and the actinides are surrounded by ten oxygen atoms from five bidentate oxalate anions. The mean metal-oxygen distances obtained by XAS measurements are in agreement with those calculated from XRD lattice parameters.

Johnston Atoll Plutonium Cleanup Project. Contract bridge report. Technical report, 1 June-5 August 1993

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hellier, C.L.; Doane, R.W.

1995-04-01

This report continues the documentation of the operation of TMA/Eberline`s Segmented Gate System technology for removing mixed plutonium and americium contamination at DNA`s Johnston Atoll site. Contaminated feed is conveyed under arrays of radiation detectors coupled with sophisticated computer software developed by Eberline Instrument Corporation. Segmented gates (chutes) on pneumatically-driven pistons move forward when contamination is detected to remove only the contaminated portion from the main flow of feed material. Only about one pint of contaminant is removed during each diversion event. At the JA site, a 98% volume reduction has been achieved, with the remediated soil cleaned to DNA`smore » criteria for release for unrestricted use of 500 Bq/kg total transuranic alpha contamination and no hot particles of greater than 5000 Becquerrels. The low level waste concentrate is expected to be packaged for shipment to an approved defense waste disposal site.« less

Thermodynamic constants for actinide oxides and oxyhydroxides relevant to actinide volatility calculations for thermal oxidation processes

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ebbinghaus, B.B.; Krikorian, O.H.

The purpose of this report is to provide input of thermodynamic data on actinide volatilities to EERC for use in their computer code for modeling of metal volatilities in incinerators. It is also anticipated that the data may be documented later in an EPA sponsored ``Metals Bible.`` It should be noted that only upper limits for the volatility of PuO{sub 2}(s) due to PuO{sub 3}(g) and PuO{sub 2}(OH){sub 2}(g) and the volatility of AmO{sub 2} in PuO{sub 2}(s) due to AmO{sub 3}(g) and AmO{sub 2}(OH){sub 2}(g) could be set. The data on the americium vapor species are intended for calculationsmore » where AmO{sub 2} is present as a solid solution in PuO{sub 2}(s).« less

Contributions of Various Radiological Sources to Background in a Suburban Environment

DOE Office of Scientific and Technical Information (OSTI.GOV)

Milvenan, Richard D.; Hayes, Robert B.

This work is a brief overview and comparison of dose rates stemming from both indoor and outdoor natural background radiation and household objects within a suburban environment in North Carolina. Combined gamma and beta dose rates were taken from indoor objects that ranged from the potassium in fruit to the americium in smoke detectors. For outdoor measurements, various height and time data samples were collected to show fluctuations in dose rate due to temperature inversion and geometric attenuation. Although each sample tested proved to have a statistically significant increase over background using Students t-test, no sample proved to be moremore » than a minor increase in natural radiation dose. Furthermore, the relative contributions from natural radioactivity such as potassium in foods and common household items are shown to be easily distinguished from background using standard handheld instrumentation when applied in a systematic, methodological manner.« less

Radioactive sample effects on EDXRF spectra

DOE Office of Scientific and Technical Information (OSTI.GOV)

Worley, Christopher G

2008-01-01

Energy dispersive X-ray fluorescence (EDXRF) is a rapid, straightforward method to determine sample elemental composition. A spectrum can be collected in a few minutes or less, and elemental content can be determined easily if there is adequate energy resolution. Radioactive alpha emitters, however, emit X-rays during the alpha decay process that complicate spectral interpretation. This is particularly noticeable when using a portable instrument where the detector is located in close proximity to the instrument analysis window held against the sample. A portable EDXRF instrument was used to collect spectra from specimens containing plutonium-239 (a moderate alpha emitter) and americium-241 (amore » heavy alpha emitter). These specimens were then analyzed with a wavelength dispersive XRF (WDXRF) instrument to demonstrate the differences to which sample radiation-induced X-ray emission affects the detectors on these two types of XRF instruments.« less

Area G perimeter surface-soil and single-stage water sampling: Environmental surveillance for fiscal year 95. Progress report

DOE Office of Scientific and Technical Information (OSTI.GOV)

Childs, M.; Conrad, R.

1997-09-01

ESH-19 personnel collected soil and single-stage water samples around the perimeter of Area G at Los Alamos National Laboratory (LANL) during FY 95 to characterize possible radionuclide movement out of Area G through surface water and entrained sediment runoff. Soil samples were analyzed for tritium, total uranium, isotopic plutonium, americium-241, and cesium-137. The single-stage water samples were analyzed for tritium and plutonium isotopes. All radiochemical data was compared with analogous samples collected during FY 93 and 94 and reported in LA-12986 and LA-13165-PR. Six surface soils were also submitted for metal analyses. These data were included with similar data generatedmore » for soil samples collected during FY 94 and compared with metals in background samples collected at the Area G expansion area.« less

Probabilistic performance-assessment modeling of the mixed waste landfill at Sandia National Laboratories.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Peace, Gerald; Goering, Timothy James; Miller, Mark Laverne

2007-01-01

A probabilistic performance assessment has been conducted to evaluate the fate and transport of radionuclides (americium-241, cesium-137, cobalt-60, plutonium-238, plutonium-239, radium-226, radon-222, strontium-90, thorium-232, tritium, uranium-238), heavy metals (lead and cadmium), and volatile organic compounds (VOCs) at the Mixed Waste Landfill (MWL). Probabilistic analyses were performed to quantify uncertainties inherent in the system and models for a 1,000-year period, and sensitivity analyses were performed to identify parameters and processes that were most important to the simulated performance metrics. Comparisons between simulated results and measured values at the MWL were made to gain confidence in the models and perform calibrations whenmore » data were available. In addition, long-term monitoring requirements and triggers were recommended based on the results of the quantified uncertainty and sensitivity analyses.« less

Element analysis and calculation of the attenuation coefficients for gold, bronze and water matrixes using MCNP, WinXCom and experimental data

NASA Astrophysics Data System (ADS)

Esfandiari, M.; Shirmardi, S. P.; Medhat, M. E.

2014-06-01

In this study, element analysis and the mass attenuation coefficient for matrixes of gold, bronze and water with various impurities and the concentrations of heavy metals (Cu, Mn, Pb and Zn) are evaluated and calculated by the MCNP simulation code for photons emitted from Barium-133, Americium-241 and sources with energies between 1 and 100 keV. The MCNP data are compared with the experimental data and WinXCom code simulated results by Medhat. The results showed that the obtained results of bronze and gold matrix are in good agreement with the other methods for energies above 40 and 60 keV, respectively. However for water matrixes with various impurities, there is a good agreement between the three methods MCNP, WinXCom and the experimental one in low and high energies.

Disposal of disused sealed radiation sources in Boreholes

DOE Office of Scientific and Technical Information (OSTI.GOV)

Vicente, R.

2007-07-01

This paper gives a description of the concept of a geological repository for disposal of disused sealed radiation sources (DSRS) under development in the Institute of Energy and Nuclear Research (IPEN), in Brazil. DSRS represent a significant fraction of total activity of radioactive wastes to be managed. Most DSRS are collected and temporarily stored at IPEN. As of 2006, the total collected activity is 800 TBq in 7,508 industrial gauge or radiotherapy sources, 7.2 TBq in about 72,000 Americium-241 sources detached from lightning rods, and about 0,5 GBq in 20,857 sources from smoke detectors. The estimated inventory of sealed sourcesmore » in the country is 2.7 hundred thousand sources with 26 PBq. The proposed repository is designed to receive the total inventory of sealed sources. A description of the pre-disposal facilities at IPEN is also presented. (authors)« less

Neutron dose per fluence and weighting factors for use at high energy accelerators

DOE Office of Scientific and Technical Information (OSTI.GOV)

Cossairt, J.Donald; Vaziri, Kamran; /Fermilab

2008-07-01

In June 2007, the United States Department of Energy incorporated revised values of neutron weighting factors into its occupational radiation protection Regulation 10 CFR Part 835 as part of updating its radiation dosimetry system. This has led to a reassessment of neutron radiation fields at high energy proton accelerators such as those at the Fermi National Accelerator Laboratory (Fermilab). Values of dose per fluence factors appropriate for accelerator radiation fields calculated elsewhere are collated and radiation weighting factors compared. The results of this revision to the dosimetric system are applied to americium-beryllium neutron energy spectra commonly used for instrument calibrations.more » A set of typical accelerator neutron energy spectra previously measured at Fermilab are reassessed in light of the new dosimetry system. The implications of this revision are found to be of moderate significance.« less

Electrically active defects in p-type silicon after alpha-particle irradiation

NASA Astrophysics Data System (ADS)

Danga, Helga T.; Auret, F. Danie; Tunhuma, Shandirai M.; Omotoso, Ezekiel; Igumbor, Emmanuel; Meyer, Walter E.

2018-04-01

In this work, we investigated the defects introduced when boron (B) doped silicon (Si) was irradiated by making use of a 5.4 MeV americium (Am) 241 foil radioactive source with a fluence rate of 7×106 cm-2 s-1 at room temperature. Deep level transient spectroscopy (DLTS) and Laplace-DLTS measurements were used to investigate the electronic properties of the introduced defects. After exposure at a fluence of 5.1×1010 cm-2, the energy levels of the hole traps measured were: H(0.10), H(0.16), H(0.33) and H(0.52) The defect level H(0.10) was tri-vacancy related. H(0.33) was identified as the interstitial carbon (Ci) related defect which was a result of radiation induced damage. H(0.52) was a B-related defect. Explicit deductions about the origin of H(0.16) have not yet been achieved.

INL DPAH STAAR 2015 Annual Report

DOE Office of Scientific and Technical Information (OSTI.GOV)

Peterman, Dean Richard

2015-09-15

Research conducted at the INL has demonstrated the synergistic extraction of americium using solvents comprised of bis(o,o-(trifluoromethyl)phenyl) dithiophosphinic acid (DPAH “1”) and trioctylphosphine oxide (TOPO), butyl bis(2,4,4-trimethylpentyl) phosphinate (BuCy272), or dibutyl butylphosphonate (DBBP). One potential drawback of this separations scheme is that soft metals such as silver, cadmium, or palladium and fission products such as zirconium are well extracted by these solvents. Several potential scrubbing reagents were examined. Of the scrubbing reagents studied, cysteine and methione exhibited some ability to scrub soft metals from the loaded solvent. More conventional scrub reagents such as ammonium fluoride or oxalic acid were notmore » effective. Reagents like Bimet and CDTA were not soluble at the acidities used in these studies. Unfortunately, these results indicate that the identification of effective scrubbing reagents for use in a flowsheet based upon the INL DPAH is going to be very difficult.« less

Silicon Carbide Radioisotope Batteries

NASA Technical Reports Server (NTRS)

Rybicki, George C.

2005-01-01

The substantial radiation resistance and large bandgap of SiC semiconductor materials makes them an attractive candidate for application in a high efficiency, long life radioisotope battery. To evaluate their potential in this application, simulated batteries were constructed using SiC diodes and the alpha particle emitter Americium Am-241 or the beta particle emitter Promethium Pm-147. The Am-241 based battery showed high initial power output and an initial conversion efficiency of approximately 16%, but the power output decayed 52% in 500 hours due to radiation damage. In contrast the Pm-147 based battery showed a similar power output level and an initial conversion efficiency of approximately 0.6%, but no degradation was observed in 500 hours. However, the Pm-147 battery required approximately 1000 times the particle fluence as the Am-242 battery to achieve a similar power output. The advantages and disadvantages of each type of battery and suggestions for future improvements will be discussed.

Rapid sequential determination of Pu, 90Sr and 241Am nuclides in environmental samples using an anion exchange and Sr-Spec resins.

PubMed

Lee, M H; Ahn, H J; Park, J H; Park, Y J; Song, K

2011-02-01

This paper presents a quantitative and rapid method of sequential separation of Pu, (90)Sr and (241)Am nuclides in environmental soil samples with an anion exchange resin and Sr Spec resin. After the sample solution was passed through an anion exchange column connected to a Sr Spec column, Pu isotopes were purified from the anion exchange column. Strontium-90 was separated from other interfering elements by the Sr Spec column. Americium-241 was purified from lanthanides by the anion exchange resin after oxalate co-precipitation. Measurement of Pu and Am isotopes was carried out using an α-spectrometer. Strontium-90 was measured by a low-level liquid scintillation counter. The radiochemical procedure of Pu, (90)Sr and (241)Am nuclides investigated in this study validated by application to IAEA reference materials and environmental soil samples. Copyright © 2010 Elsevier Ltd. All rights reserved.

Environmental aspects of the transuranics: a selected, annotated bibliography. [Pu-238, Pu-239

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ensminger, J.T.; Martin, F.M.; Fore, C.S.

This eighth published bibliography of 427 references is compiled from the Nevada Applied Ecology Information Center's Data Base on the Environmental Aspects of the Transuranics. The data base was built to provide information support to the Nevada Applied Ecology Group (NAEG) of ERDA's Nevada Operations Office. The general scope covers environmental aspects of uranium and the transuranic elements, with emphasis on plutonium. This bibliography highlights literature on plutonium 238 and 239 and americium in the critical organs of man and animals. Supporting information on ecology of the Nevada Test Site and reviews and summarizing literature on other radionuclides have beenmore » included at the request of the NAEG. The references are arranged by subject category with leading authors appearing alphabetically in each category. Indexes are provided for author(s), geographic location, keyword(s), taxon, title, and publication description.« less

Method of uranium reclamation from aqueous systems by reactive ion exchange. [US DOE patent application; anion exchange resin of copolymerized divinyl-benzene and styrene having quarternary ammonium groups and bicarbonate ligands

DOEpatents

Maya, L.

1981-11-05

A reactive ion exchange method for separation and recovery of values of uranium, neptunium, plutonium, or americium from substantially neutral aqueous systems of said metals comprises contacting said system with an effective amount of a basic anion exchange resin of copolymerized divinyl-benzene and styrene having quarternary ammonium groups and bicarbonate ligands to achieve nearly 100% sorption of said actinyl ion onto said resin and an aqueous system practically free of said actinyl ions. The method is operational over an extensive range of concentrations from about 10/sup -6/ M to 1.0 M actinyl ion and a pH range of about 4 to 7. The method has particulr application to treatment of waste streams from Purex-type nuclear fuel reprocessing facilities and hydrometallurgical processes involving U, Np, P, or Am.

LIBS Spectral Data for a Mixed Actinide Fuel Pellet Containing Uranium, Plutonium, Neptunium and Americium

DOE Office of Scientific and Technical Information (OSTI.GOV)

Judge, Elizabeth J.; Berg, John M.; Le, Loan A.

2012-06-18

Laser-induced breakdown spectroscopy (LIBS) was used to analyze a mixed actinide fuel pellet containing 75% UO{sub 2}/20% PuO{sub 2}/3% AmO{sub 2}/2% NpO{sub 2}. The preliminary data shown here is the first report of LIBS analysis of a mixed actinide fuel pellet, to the authors knowledge. The LIBS spectral data was acquired in a plutonium facility at Los Alamos National Laboratory where the sample was contained within a glove box. The initial installation of the glove box was not intended for complete ultraviolet (UV), visible (VIS) and near infrared (NIR) transmission, therefore the LIBS spectrum is truncated in the UV andmore » NIR regions due to the optical transmission of the window port and filters that were installed. The optical collection of the emission from the LIBS plasma will be optimized in the future. However, the preliminary LIBS data acquired is worth reporting due to the uniqueness of the sample and spectral data. The analysis of several actinides in the presence of each other is an important feature of this analysis since traditional methods must chemically separate uranium, plutonium, neptunium, and americium prior to analysis. Due to the historic nature of the sample fuel pellet analyzed, the provided sample composition of 75% UO{sub 2}/20% PuO{sub 2}/3% AmO{sub 2}/2% NpO{sub 2} cannot be confirm without further analytical processing. Uranium, plutonium, and americium emission lines were abundant and easily assigned while neptunium was more difficult to identify. There may be several reasons for this observation, other than knowing the exact sample composition of the fuel pellet. First, the atomic emission wavelength resources for neptunium are limited and such techniques as hollow cathode discharge lamp have different dynamics than the plasma used in LIBS which results in different emission spectra. Secondly, due to the complex sample of four actinide elements, which all have very dense electronic energy levels, there may be reactions and interactions occurring within the plasma, such as collisional energy transfer, that might be a factor in the reduction in neptunium emission lines. Neptunium has to be analyzed alone using LIBS to further understand the dynamics that may be occurring in the plasma of the mixed actinide fuel pellet sample. The LIBS data suggests that the emission spectrum for the mixed actinide fuel pellet is not simply the sum of the emission spectra of the pure samples but is dependent on the species present in the plasma and the interactions and reactions that occur within the plasma. Finally, many of the neptunium lines are in the near infrared region which is drastically reduced in intensity by the current optical setup and possibly the sensitivity of the emission detector in the spectral region. Once the optics are replaced and the optical collection system is modified and optimized, the probability of observing emission lines for neptunium might be increased significantly. The mixed actinide fuel pellet was analyzed under the experimental conditions listed in Table 1. The LIBS spectra of the fuel pellet are shown in Figures 1-49. The spectra are labeled with the observed wavelength and atomic species (both neutral (I) and ionic (II)). Table 2 is a complete list of the observed and literature based emission wavelengths. The literature wavelengths have references including NIST Atomic Spectra Database (NIST), B.A. Palmer et al. 'An Atlas of Uranium Emission Intensities in a Hollow Cathode Discharge' taken at the Kitt Peak National Observatory (KPNO), R.L. Kurucz 1995 Atomic Line Data from the Smithsonian Astrophysical Observatory (SAO), J. Blaise et al. 'The Atomic Spectrum of Plutonium' from Argonne National Laboratory (BFG), and M. Fred and F.S. Tomkins, 'Preliminary Term Analysis of Am I and Am II Spectra' (FT). The dash (-) shown under Ionic State indicates that the ionic state of the transition was not available. In the spectra, the dash (-) is replaced with a question mark (?). Peaks that are not assigned are most likely real features and not noise but cannot be confidently assigned to a transition without further investigation. Several peaks have multiple assignments due to limited resolution of the spectrometer used (20,000, {lambda}/{Delta}{lambda}) and without the availability, at this point in time, of pure PuO{sub 2}, AmO{sub 2}, and NpO{sub 2} to confirm the identity of the peaks. A different spectrometer was used in the plutonium facility to collect the mixed actinide fuel pellet data (Echelle 3000) than the DUO{sub 2}, ThO{sub 2} and uranium ore previously reported [6-8] (Echelle 4000) which accounts for the slight shift in the observed wavelength of the uranium emission lines.« less

Lower thresholds for lifetime health effects in mammals from high-LET radiation - Comparison with chronic low-LET radiation.

PubMed

Sazykina, Tatiana G; Kryshev, Alexander I

2016-12-01

Lower threshold dose rates and confidence limits are quantified for lifetime radiation effects in mammalian animals from internally deposited alpha-emitting radionuclides. Extensive datasets on effects from internal alpha-emitters are compiled from the International Radiobiological Archives. In total, the compiled database includes 257 records, which are analyzed by means of non-parametric order statistics. The generic lower threshold for alpha-emitters in mammalian animals (combined datasets) is 6.6·10 -5  Gy day -1 . Thresholds for individual alpha-emitting elements differ considerably: plutonium and americium - 2.0·10 -5  Gy day -1 ; radium - 2.1·10 -4  Gy day -1 . Threshold for chronic low-LET radiation is previously estimated at 1·10 -3  Gy day -1 . For low exposures, the following values of alpha radiation weighting factor w R for internally deposited alpha-emitters in mammals are quantified: w R (α) = 15 as a generic value for the whole group of alpha-emitters; w R (Pu) = 50 for plutonium; w R (Am) = 50 for americium; w R (Ra) = 5 for radium. These values are proposed to serve as radiation weighting factors in calculations of equivalent doses to non-human biota. The lower threshold dose rate for long-lived mammals (dogs) is significantly lower than comparing with the threshold for short-lived mammals (mice): 2.7·10 -5  Gy day -1 , and 2.0·10 -4  Gy day -1 , respectively. The difference in thresholds is exactly reflecting the relationship between the natural longevity of these two species. Graded scale of severity in lifetime radiation effects in mammals is developed, based on compiled datasets. Being placed on the severity scale, the effects of internal alpha-emitters are situated in the zones of considerably lower dose rates than effects of the same severity caused by low-LET radiation. RBE values, calculated for effects of equal severity, are found to depend on the intensity of chronic exposure: different RBE values are characteristic for low, moderate, and high lifetime exposures (30, 70, and 13, respectively). The results of the study provide a basis for selecting correct values of radiation weighting factors in dose assessment to non-human biota. Copyright © 2016 Elsevier Ltd. All rights reserved.

Response of Microbial Community Function to Fluctuating Geochemical Conditions within a Legacy Radioactive Waste Trench Environment

PubMed Central

Kinsela, Andrew S.; Bligh, Mark W.; Harrison, Jennifer J.; Payne, Timothy E.

2017-01-01

ABSTRACT During the 1960s, small quantities of radioactive materials were codisposed with chemical waste at the Little Forest Legacy Site (Sydney, Australia) in 3-meter-deep, unlined trenches. Chemical and microbial analyses, including functional and taxonomic information derived from shotgun metagenomics, were collected across a 6-week period immediately after a prolonged rainfall event to assess the impact of changing water levels upon the microbial ecology and contaminant mobility. Collectively, results demonstrated that oxygen-laden rainwater rapidly altered the redox balance in the trench water, strongly impacting microbial functioning as well as the radiochemistry. Two contaminants of concern, plutonium and americium, were shown to transition from solid-iron-associated species immediately after the initial rainwater pulse to progressively more soluble moieties as reducing conditions were enhanced. Functional metagenomics revealed the potentially important role that the taxonomically diverse microbial community played in this transition. In particular, aerobes dominated in the first day, followed by an increase of facultative anaerobes/denitrifiers at day 4. Toward the mid-end of the sampling period, the functional and taxonomic profiles depicted an anaerobic community distinguished by a higher representation of dissimilatory sulfate reduction and methanogenesis pathways. Our results have important implications to similar near-surface environmental systems in which redox cycling occurs. IMPORTANCE The role of chemical and microbiological factors in mediating the biogeochemistry of groundwaters from trenches used to dispose of radioactive materials during the 1960s is examined in this study. Specifically, chemical and microbial analyses, including functional and taxonomic information derived from shotgun metagenomics, were collected across a 6-week period immediately after a prolonged rainfall event to assess how changing water levels influence microbial ecology and contaminant mobility. Results demonstrate that oxygen-laden rainwater rapidly altered the redox balance in the trench water, strongly impacting microbial functioning as well as the radiochemistry. Two contaminants of concern, plutonium and americium, were shown to transition from solid-iron-associated species immediately after the initial rainwater pulse to progressively more soluble moieties as reducing conditions were enhanced. Functional metagenomics revealed the important role that the taxonomically diverse microbial community played in this transition. Our results have important implications to similar near-surface environmental systems in which redox cycling occurs. PMID:28667104

Response of Microbial Community Function to Fluctuating Geochemical Conditions within a Legacy Radioactive Waste Trench Environment.

PubMed

Vázquez-Campos, Xabier; Kinsela, Andrew S; Bligh, Mark W; Harrison, Jennifer J; Payne, Timothy E; Waite, T David

2017-09-01

During the 1960s, small quantities of radioactive materials were codisposed with chemical waste at the Little Forest Legacy Site (Sydney, Australia) in 3-meter-deep, unlined trenches. Chemical and microbial analyses, including functional and taxonomic information derived from shotgun metagenomics, were collected across a 6-week period immediately after a prolonged rainfall event to assess the impact of changing water levels upon the microbial ecology and contaminant mobility. Collectively, results demonstrated that oxygen-laden rainwater rapidly altered the redox balance in the trench water, strongly impacting microbial functioning as well as the radiochemistry. Two contaminants of concern, plutonium and americium, were shown to transition from solid-iron-associated species immediately after the initial rainwater pulse to progressively more soluble moieties as reducing conditions were enhanced. Functional metagenomics revealed the potentially important role that the taxonomically diverse microbial community played in this transition. In particular, aerobes dominated in the first day, followed by an increase of facultative anaerobes/denitrifiers at day 4. Toward the mid-end of the sampling period, the functional and taxonomic profiles depicted an anaerobic community distinguished by a higher representation of dissimilatory sulfate reduction and methanogenesis pathways. Our results have important implications to similar near-surface environmental systems in which redox cycling occurs. IMPORTANCE The role of chemical and microbiological factors in mediating the biogeochemistry of groundwaters from trenches used to dispose of radioactive materials during the 1960s is examined in this study. Specifically, chemical and microbial analyses, including functional and taxonomic information derived from shotgun metagenomics, were collected across a 6-week period immediately after a prolonged rainfall event to assess how changing water levels influence microbial ecology and contaminant mobility. Results demonstrate that oxygen-laden rainwater rapidly altered the redox balance in the trench water, strongly impacting microbial functioning as well as the radiochemistry. Two contaminants of concern, plutonium and americium, were shown to transition from solid-iron-associated species immediately after the initial rainwater pulse to progressively more soluble moieties as reducing conditions were enhanced. Functional metagenomics revealed the important role that the taxonomically diverse microbial community played in this transition. Our results have important implications to similar near-surface environmental systems in which redox cycling occurs. Copyright © 2017 Vázquez-Campos et al.

Insight into the Extraction Mechanism of Americium(III) over Europium(III) with Pyridylpyrazole: A Relativistic Quantum Chemistry Study.

PubMed

Kong, Xiang-He; Wu, Qun-Yan; Wang, Cong-Zhi; Lan, Jian-Hui; Chai, Zhi-Fang; Nie, Chang-Ming; Shi, Wei-Qun

2018-05-10

Separation of trivalent actinides (An(III)) and lanthanides (Ln(III)) is one of the most important steps in spent nuclear fuel reprocessing. However, it is very difficult and challenging to separate them due to their similar chemical properties. Recently the pyridylpyrazole ligand (PypzH) has been identified to show good separation ability toward Am(III) over Eu(III). In this work, to explore the Am(III)/Eu(III) separation mechanism of PypzH at the molecular level, the geometrical structures, bonding nature, and thermodynamic behaviors of the Am(III) and Eu(III) complexes with PypzH ligands modified by alkyl chains (Cn-PypzH, n = 2, 4, 8) have been systematically investigated using scalar relativistic density functional theory (DFT). According to the NBO (natural bonding orbital) and QTAIM (quantum theory of atoms in molecules) analyses, the M-N bonds exhibit a certain degree of covalent character, and more covalency appears in Am-N bonds compared to Eu-N bonds. Thermodynamic analyses suggest that the 1:1 extraction reaction, [M(NO 3 )(H 2 O) 6 ] 2+ + PypzH + 2NO 3 - → M(PypzH)(NO 3 ) 3 (H 2 O) + 5H 2 O, is the most suitable for Am(III)/Eu(III) separation. Furthermore, the extraction ability and the Am(III)/Eu(III) selectivity of the ligand PypzH is indeed enhanced by adding alkyl-substituted chains in agreement with experimental observations. Besides this, the nitrogen atom of pyrazole ring plays a more significant role in the extraction reactions related to Am(III)/Eu(III) separation compared to that of pyridine ring. This work could identify the mechanism of the Am(III)/Eu(III) selectivity of the ligand PypzH and provide valuable theoretical information for achieving an efficient Am(III)/Eu(III) separation process for spent nuclear fuel reprocessing.

How Do Radionuclides Accumulate in Marine Organisms? A Case Study of Europium with Aplysina cavernicola

DOE PAGES

Maloubier, Melody; Shuh, David K.; Minasian, Stefan G.; ...

2016-09-15

In the ocean, complex interactions between natural and anthropogenic radionuclides, seawater, and diverse marine biota provide a unique window through which to examine ecosystem and trophic transfer mechanisms in cases of accidental dissemination. The nature of interaction between radionuclides, the marine environment, and marine species is therefore essential for better understanding transfer mechanisms from the hydrosphere to the biosphere. Although data pertaining to the rate of global transfer are often available, little is known regarding the mechanism of environmental transport and uptake of heavy radionuclides by marine species. Among marine species, sponges are immobile active filter feeders and have beenmore » identified as hyperaccumulators of several heavy metals. We have selected the Mediterranean sponge Aplysina cavernicola as a model species for this study. Actinide elements are not the only source of radioactive release in cases of civilian nuclear events; however, their physicochemical transfer mechanisms to marine species remain largely unknown. We have targeted europium(III) as a representative of the trivalent actinides such as americium or curium. To unravel biological uptake mechanisms of europium in A. cavernicola, we have combined radiometric (γ) measurements with spectroscopic (time-resolved laser-induced fluorescence spectroscopy, TRLIFS, and X-ray absorption near-edge structure, XANES) and imaging (transmission electron microscopy, TEM, and scanning transmission X-ray microscopy, STXM) techniques. Here, we have observed that the colloids of NaEu(CO 3) 2 ·nH 2O formed in seawater are taken up by A. cavernicola with no evidence that lethal dose has been reached in our working conditions. Spectroscopic results suggest that there is no change of speciation during uptake. Finally, TEM and STXM images recorded at different locations across a sponge cross section, together with differential cell separation, indicate the presence of europium particles (around 200 nm) mainly located in the skeleton and toward the outer surface of the sponge.« less

How Do Radionuclides Accumulate in Marine Organisms? A Case Study of Europium with Aplysina cavernicola

DOE Office of Scientific and Technical Information (OSTI.GOV)

Maloubier, Melody; Shuh, David K.; Minasian, Stefan G.

In the ocean, complex interactions between natural and anthropogenic radionuclides, seawater, and diverse marine biota provide a unique window through which to examine ecosystem and trophic transfer mechanisms in cases of accidental dissemination. The nature of interaction between radionuclides, the marine environment, and marine species is therefore essential for better understanding transfer mechanisms from the hydrosphere to the biosphere. Although data pertaining to the rate of global transfer are often available, little is known regarding the mechanism of environmental transport and uptake of heavy radionuclides by marine species. Among marine species, sponges are immobile active filter feeders and have beenmore » identified as hyperaccumulators of several heavy metals. We have selected the Mediterranean sponge Aplysina cavernicola as a model species for this study. Actinide elements are not the only source of radioactive release in cases of civilian nuclear events; however, their physicochemical transfer mechanisms to marine species remain largely unknown. We have targeted europium(III) as a representative of the trivalent actinides such as americium or curium. To unravel biological uptake mechanisms of europium in A. cavernicola, we have combined radiometric (γ) measurements with spectroscopic (time-resolved laser-induced fluorescence spectroscopy, TRLIFS, and X-ray absorption near-edge structure, XANES) and imaging (transmission electron microscopy, TEM, and scanning transmission X-ray microscopy, STXM) techniques. Here, we have observed that the colloids of NaEu(CO 3) 2 ·nH 2O formed in seawater are taken up by A. cavernicola with no evidence that lethal dose has been reached in our working conditions. Spectroscopic results suggest that there is no change of speciation during uptake. Finally, TEM and STXM images recorded at different locations across a sponge cross section, together with differential cell separation, indicate the presence of europium particles (around 200 nm) mainly located in the skeleton and toward the outer surface of the sponge.« less

Rapid determination of alpha emitters using Actinide resin.

PubMed

Navarro, N; Rodriguez, L; Alvarez, A; Sancho, C

2004-01-01

The European Commission has recently published the recommended radiological protection criteria for the clearance of building and building rubble from the dismantling of nuclear installations. Radionuclide specific clearance levels for actinides are very low (between 0.1 and 1 Bq g(-1)). The prevalence of natural radionuclides in rubble materials makes the verification of these levels by direct alpha counting impossible. The capability of Actinide resin (Eichrom Industries, Inc.) for extracting plutonium and americium from rubble samples has been tested in this work. Besides a strong affinity for actinides in the tri, tetra and hexavalent oxidation states, this extraction chromatographic resin presents an easy recovery of absorbed radionuclides. The retention capability was evaluated on rubble samples spiked with certified radionuclide standards (239Pu and 241Am). Samples were leached with nitric acid, passed through a chromatographic column containing the resin and the elution fraction was measured by LSC. Actinide retention varies from 60% to 80%. Based on these results, a rapid method for the verification of clearance levels for actinides in rubble samples is proposed.

Nuclear and radiological terrorism: continuing education article.

PubMed

Anderson, Peter D; Bokor, Gyula

2013-06-01

Terrorism involving radioactive materials includes improvised nuclear devices, radiation exposure devices, contamination of food sources, radiation dispersal devices, or an attack on a nuclear power plant or a facility/vehicle that houses radioactive materials. Ionizing radiation removes electrons from atoms and changes the valence of the electrons enabling chemical reactions with elements that normally do not occur. Ionizing radiation includes alpha rays, beta rays, gamma rays, and neutron radiation. The effects of radiation consist of stochastic and deterministic effects. Cancer is the typical example of a stochastic effect of radiation. Deterministic effects include acute radiation syndrome (ARS). The hallmarks of ARS are damage to the skin, gastrointestinal tract, hematopoietic tissue, and in severe cases the neurovascular structures. Radiation produces psychological effects in addition to physiological effects. Radioisotopes relevant to terrorism include titrium, americium 241, cesium 137, cobalt 60, iodine 131, plutonium 238, califormium 252, iridium 192, uranium 235, and strontium 90. Medications used for treating a radiation exposure include antiemetics, colony-stimulating factors, antibiotics, electrolytes, potassium iodine, and chelating agents.

A Plutonium-Contaminated Wound, 1985, USA

DOE Office of Scientific and Technical Information (OSTI.GOV)

Doran M. Christensen, DO, REAC /TS Associate Director and Staff Physician Eugene H. Carbaugh, CHP, Staff Scientist, Internal Dosimetry Manager, Pacific Northwest National Laboratory, Richland, Washington

2012-02-02

A hand injury occurred at a U.S. facility in 1985 involving a pointed shaft (similar to a meat thermometer) that a worker was using to remove scrap solid plutonium from a plastic bottle. The worker punctured his right index finger on the palm side at the metacarpal-phalangeal joint. The wound was not through-and- through, although it was deep. The puncture wound resulted in deposition of ~48 kBq of alpha activity from the weapons-grade plutonium mixture with a nominal 12 to 1 Pu-alpha to {sup 241}Am-alpha ratio. This case clearly showed that DTPA was very effective for decorporation of plutonium andmore » americium. The case is a model for management of wounds contaminated with transuranics: (1) a team approach for dealing with all of the issues surrounding the incident, including the psychological, (2) early surgical intervention for foreign-body removal, (3) wound irrigation with DTPA solution, and (4) early and prolonged DTPA administration based upon bioassay and in vivo dosimetry.« less

Neutron capture and neutron-induced fission experiments on americium isotopes with DANCE

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jandel, M.; Bredeweg, T. A.; Fowler, M. M.

2009-01-28

Neutron capture cross section data on Am isotopes were measured using the Detector for Advanced Neutron Capture Experiments (DANCE) at Los Alamos National Laboratory. The neutron capture cross section was determined for {sup 241}Am for neutron energies between thermal and 320 keV. Preliminary results were also obtained for {sup 243}Am for neutron energies between 10 eV and 250 keV. The results on concurrent neutron-induced fission and neutron-capture measurements on {sup 242m}Am will be presented where the fission events were actively triggered during the experiments. In these experiments, a Parallel-Plate Avalanche Counter (PPAC) detector that surrounds the target located in themore » center of the DANCE array was used as a fission-tagging detector to separate (n,{gamma}) events from (n,f) events. The first direct observation of neutron capture on {sup 242m}Am in the resonance region in between 2 and 9 eV of the neutron energy was obtained.« less

Neutron capture and neutron-induced fission experiments on americium isotopes with DANCE

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jandel, Marian

2008-01-01

Neutron capture cross section data on Am isotopes were measured using the Detector for Advanced Neutron Capture Experiments (DANCE) at Los Alamos National Laboratory. The neutron capture cross section was determined for {sup 241}Am for neutron energies between thermal and 320 keV. Preliminary results were also obtained for {sup 243}Am for neutron energies between 35 eV and 200 keV. The results on concurrent neutron-induced fission and neutron-capture measurements on {sup 242m}Am will be presented, where the fission events were actively triggered during the experiments. In these experiments, the Parallel-Plate Avalanche Counter (PPAC) detector that surrounds the target located in themore » center of the DANCE array was used as a fission-tagging detector to separate (n,{gamma}) from (n,f) events. The first evidence of neutron capture on {sup 242m}Am in the resonance region in between 2 and 9 eV of the neutron energy was obtained.« less

Johnston Atoll Plutonium Cleanup Project, plant modification and operation. Volume 1. Annual report option year 2. Technical report, 1 October 1992-24 May 1993

DOE Office of Scientific and Technical Information (OSTI.GOV)

Moroney, K.S.; Moroney, J.D.; Johnson, N.R.

1995-04-01

This report continues the documentation of the operation of TMA/Eberline`s Segmented Gate System technology for removing mixed plutonium and americium contamination at DNA`s Johnston Atoll site. Contaminated feed is conveyed under arrays of radiation detectors coupled with sophisticated computer software developed by Eberline Instrument Corporation. Segmented gates (chutes) on pneumatically-driven pistons move forward when contamination is detected to remove only the contaminated portion from the main flow of feed material. Only about one pint of contaminant is removed during each diversion event. At the JA site, a 98% volume reduction has been achieved, with the remediated soil cleaned to DNA`smore » criteria for release for unrestricted use of 500 Bq/kg total tnansuranic alpha contamination and no hot particles of greater than 5000 Becquerrels. The low level waste concentrate is expected to be packaged for shipment to an approved defense waste disposal site.« less

Johnston Atoll Plutonium Cleanup Project. Plant modification and operation. Volume 2. Annual report option year 2. Appendix A. Technical report, 1 October 1992-24 May 1993

DOE Office of Scientific and Technical Information (OSTI.GOV)

Moroney, K.S.; Moroney, J.D.; Johnson, N.R.

1995-04-01

This report continues the documentation of the operation of TMA/Eberline`s Segmented Gate System technology for removing mixed plutonium and americium contamination at DNA`s Johnston Atoll site. Contaminated feed is conveyed under arrays of radiation detectors coupled with sophisticated computer software developed by Eberline Instrument Corporation. Segmented gates (chutes) on pneumatically-driven pistons move forward when contamination is detected to remove only the contaminated portion from the main flow of feed material. Only about one pint of contaminant is removed during each diversion event. At the JA site, a 98% volume reduction has been achieved, with the remediated soil cleaned to DNA`smore » criteria for release for unrestricted use of 500 Bq/kg total transuranic alpha contamination and no hot particles of greater than 5000 Becquerrels. The low level waste concentrate is expected to be packaged for shipment to an approved defense waste disposal site.« less

Johnston Atoll Plutonium Cleanup Project, plant modification and operation. Volume 3. Annual report option year 2. Appendices b through h. Technical report, 1 October 1992-24 May 1993

DOE Office of Scientific and Technical Information (OSTI.GOV)

Moroney, K.S.; Moroney, J.D.; Johnson, N.R.

1995-04-01

This report continues the documentation of the operation of TMA/Eberline`s Segmented Gate System technology for removing mixed plutonium and americium contamination at DNA`s Johnston Atoll site. Contaminated feed is conveyed under arrays of radiation detectors coupled with sophisticated computer software developed by Eberline Instrument Corporation. Segmented gates (chutes) on pneumatically-driven pistons move forward when contamination is detected to remove only the contaminated portion from the main flow of feed material. Only about one pint of contaminant is removed during each diversion event. At the JA site, a 98% volume reduction has been achieved, with the remediated soil cleaned to DNA`smore » criteria for release for unrestricted use of 500 Bq/kg total transuranic alpha contamination and no hot particles of greater than 5000 Becquerrels. The low level waste concentrate is expected to be packaged for shipment to an approved defense waste disposal site.« less

Application of inductively coupled plasma sector field mass spectrometry for low-level environmental americium-241 analysis.

PubMed

Varga, Zsolt

2007-03-28

An improved and novel sample preparation method for (241)Am analysis by inductively coupled plasma sector field mass spectrometry has been developed. The procedure involves a selective CaF(2) pre-concentration followed by an extraction chromatographic separation using TRU resin. The achieved absolute detection limit of 0.86 fg (0.11 mBq) is comparable to that of alpha spectrometry (0.1 mBq) and suitable for low-level environmental measurements. Analysis of different kinds of environmental standard reference materials (IAEA-384--Fangataufa lagoon sediment, IAEA-385--Irish Sea sediment and IAEA-308--Mixed seaweed from the Mediterranean Sea) and alpha spectrometry were used to validate the procedure. The chemical recovery of sample preparation ranged between 72 and 94%. The results obtained are in good agreement with reference values and those measured by alpha spectrometry. The proposed method offers a rapid and less labor-intensive possibility for environmental (241)Am analysis than the conventionally applied radioanalytical techniques.

An In Situ Radiological Survey of Three Canyons at the Los Alamos National Laboratory

DOE Office of Scientific and Technical Information (OSTI.GOV)

R.J. Maurer

1999-06-01

An in situ radiological survey of Mortandad, Ten Site, and DP Canyons at the Los Alamos National Laboratory was conducted during August 19-30, 1996. The purpose of this survey was to measure the quantities of radionuclides that remain in the canyons from past laboratory operations. A total of 65 in situ measurements were conducted using high-resolution gamma radiation detectors at 1 meter above the ground. The measurements were obtained in the streambeds of the canyons beginning near the water-release points at the laboratories and extending to the ends of the canyons. Three man-made gamma-emitting radionuclides were detected in the canyons:more » americium-241 ({sup 241}Am), cesium-137 ({sup 137}Cs), and cobalt-60 ({sup 60}Co). Estimated contamination levels ranged from 13.3-290.4 picocuries per gram (pCi/g)for {sup 241}Am, 4.4-327.8 pCi/g for {sup 137}Cs, and 0.4-2.6 pCi/g for {sup 60}Co.« less

Effects of Organic Acids and Sylvite on Phytoextraction of 241Am Contaminated Soil.

PubMed

Wang, Ping; Du, Liang; Tan, Zhaoyi; Su, Rongbo; Li, Taowen

2017-03-01

Contamination of soil with Americium ( 241 Am) at nuclear sites in China poses a serious problem. We screened six plants, from five families, for their 241 Am-enrichment potential. Europium (Eu), which is morphologically and chemically similar to the highly toxic 241 Am, was used in its place. Moreover, the effects of sylvite, citric acid (CA), malic acid (MA), and humic acid (HA) on the absorption of 241 Am by the plants, and its transport within them, were evaluated along with their effect on plant biomass and 241 Am extraction volume. Barley and cabbage showed relatively stronger Eu accumulation capacities. Citric acid promoted the absorption of 241 Am by barley roots and its transport within the plants. The effects of sylvite were not obvious and those of HA were the weakest in case of sunflower; HA, however, maximally increased the biomass of the plants. Our results could provide the basis for future radionuclide phytoremediation of contaminated soils.

Influence of the bystander phenomenon on the chromosome aberration pattern in human lymphocytes induced by in vitro alpha-particle exposure.

PubMed

Schmid, Ernst; Roos, H

2009-04-01

A recent publication on both chromosome-type and chromatid-type aberrations in lymphocytes of patients during treatment with radium-224 for ankylosing spondilitis has revived the question of whether the chromatid-type aberrations may be the consequence of factors released by irradiated cells. Therefore, the aim of the present study was to investigate the influence of such a bystander phenomenon on the chromosome aberration pattern of lymphocytes. Monolayers of human lymphocytes were irradiated with 1 Gy of alpha-particles from an americium-241 source in the absence or presence of whole blood, autologous plasma or culture medium. In the presence of any liquid covering the monolayer during irradiation, the chromatid-type aberrations were, contrary to expectation, elevated. Whereas the intercellular distribution of dicentrics was significantly overdispersed, the chromatid-type aberrations showed a regular dispersion. It can be concluded that the enhanced frequency of chromatid aberrations is the result of a damage signal or a bystander phenomenon released by irradiated cells.

Irradiation of the Crude Venom of Bothrops jararacussu to Obtain Toxoid

NASA Astrophysics Data System (ADS)

Ferreira, Camila G.; Avalloni, Tânia M.; Oshima-Franco, Yoko; de J. Oliveira, Sara; de Oliveira, José M.; Cogo, José C.

2011-08-01

The aim of this work was to reduce the toxicity of Bothrops jararacussu venom using gamma-rays of low-energy coming from a source of Americium-241 (E = 59.6 keV and 3.7×109 Bq of activity) in order to obtain a toxoid. The radiation dose that each sample received was controlled by exposure time of the venom to the radiation beam. Mouse nerve phrenic-diaphragm preparation was used for testing the loss of venom toxicity, since the venom causes an irreversible neuromuscular blockade. In this condition, the several samples of irradiated venom, when assayed in neuromuscular preparation showed that with a dose of 0.051 Gy the paralysis caused by the irradiated venom was of 91%, at 0.360 Gy was of 79%, at 1.662 Gy was of 50% and at 2.448 Gy was of 42%. Therefore, it can be concluded that the irradiation model was able to induce a progressive loss of the venom toxicity.

Technical basis for the use of a correlated neutron source in the uranium neutron coincidence collar

DOE PAGES

Root, Margaret A.; Menlove, Howard Olsen; Lanza, Richard C.; ...

2017-01-16

Active neutron coincidence systems are commonly used by international inspectorates to verify a material balance across the various stages of the nuclear fuel cycle. The Uranium Neutron Coincidence Collar (UNCL) is one such instrument; it is used to measure the linear density of 235U (g 235U/cm of active length in assembly) in fresh light water reactor fuel in nuclear fuel fabrication facilities. The UNCL and other active neutron interrogation detectors have historically relied on americium lithium ( 241AmLi) sources to induce fission within the sample in question. Californium-252 is under consideration as a possible alternative to the traditional 241AmLi source.more » Finally, this work relied upon a combination of experiments and Monte Carlo simulations to demonstrate the technical basis for the replacement of 241AmLi sources with 252Cf sources by evaluating the statistical uncertainty in the measurements incurred by each source and assessing the penetrability of neutrons from each source for the UNCL.« less

Fifty years since the nuclear accident in Palomares (Almeria). Medical repercussions.

PubMed

Laynez-Bretones, F; Lozano-Padilla, C

In January 1966, 2 US military aircraft collided over the skies of Palomares (Almeria). One of them carried thermonuclear bombs, which released plutonium and other radioactive materials upon striking the ground. The most contaminated earth and plants were immediately removed. The Indalo Project was launched to study the effects of nuclear material on the inhabitants and environment of Palomares. A total of 1,077 inhabitants have been monitored since then, and the official version is that the ionising radiation has not been related to any type of disease. However, secrecy has surrounded much of the investigations, and no trustworthy epidemiological study has been conducted in the area. Approximately 500g of plutonium and americium remains in Palomares. Although the risk for the population appears to be low, this radioactive material should be removed as soon as possible. Copyright © 2017 Elsevier España, S.L.U. and Sociedad Española de Medicina Interna (SEMI). All rights reserved.

Methods and Models of the Hanford Internal Dosimetry Program, PNNL-MA-860

DOE Office of Scientific and Technical Information (OSTI.GOV)

Carbaugh, Eugene H.; Bihl, Donald E.; Maclellan, Jay A.

2009-09-30

The Hanford Internal Dosimetry Program (HIDP) provides internal dosimetry support services for operations at the Hanford Site. The HIDP is staffed and managed by the Radiation and Health Technology group, within the Pacific Northwest National Laboratory (PNNL). Operations supported by the HIDP include research and development, the decontamination and decommissioning of facilities formerly used to produce and purify plutonium, and waste management activities. Radioelements of particular interest are plutonium, uranium, americium, tritium, and the fission and activation product radionuclides 137Cs, 90Sr, and 60Co. This manual describes the technical basis for the design of the routine bioassay monitoring program and formore » assessment of internal dose. The purposes of the manual are as follows: • Provide assurance that the HIDP derives from a sound technical base. • Promote the consistency and continuity of routine program activities. • Provide a historical record. • Serve as a technical reference for radiation protection personnel. • Aid in identifying and planning for future needs.« less

Technical basis for the use of a correlated neutron source in the uranium neutron coincidence collar

DOE Office of Scientific and Technical Information (OSTI.GOV)

Root, Margaret A.; Menlove, Howard Olsen; Lanza, Richard C.

Active neutron coincidence systems are commonly used by international inspectorates to verify a material balance across the various stages of the nuclear fuel cycle. The Uranium Neutron Coincidence Collar (UNCL) is one such instrument; it is used to measure the linear density of 235U (g 235U/cm of active length in assembly) in fresh light water reactor fuel in nuclear fuel fabrication facilities. The UNCL and other active neutron interrogation detectors have historically relied on americium lithium ( 241AmLi) sources to induce fission within the sample in question. Californium-252 is under consideration as a possible alternative to the traditional 241AmLi source.more » Finally, this work relied upon a combination of experiments and Monte Carlo simulations to demonstrate the technical basis for the replacement of 241AmLi sources with 252Cf sources by evaluating the statistical uncertainty in the measurements incurred by each source and assessing the penetrability of neutrons from each source for the UNCL.« less

Rapid fusion method for the determination of Pu, Np, and Am in large soil samples

DOE PAGES

Maxwell, Sherrod L.; Culligan, Brian; Hutchison, Jay B.; ...

2015-02-14

A new rapid sodium hydroxide fusion method for the preparation of 10-20 g soil samples has been developed by the Savannah River National Laboratory (SRNL). The method enables lower detection limits for plutonium, neptunium, and americium in environmental soil samples. The method also significantly reduces sample processing time and acid fume generation compared to traditional soil digestion techniques using hydrofluoric acid. Ten gram soil aliquots can be ashed and fused using the new method in 1-2 hours, completely dissolving samples, including refractory particles. Pu, Np and Am are separated using stacked 2mL cartridges of TEVA and DGA Resin and measuredmore » using alpha spectrometry. The method can be adapted for measurement by inductively-coupled plasma mass spectrometry (ICP-MS). Two 10 g soil aliquots of fused soil may be combined prior to chromatographic separations to further improve detection limits. Total sample preparation time, including chromatographic separations and alpha spectrometry source preparation, is less than 8 hours.« less

High Pressure Phase Transformations in Heavy Rare Earth Metals and Connections to Actinide Crystal Structures

DOE Office of Scientific and Technical Information (OSTI.GOV)

Vohra, Yogesh K.; Sangala, Bagvanth Reddy; Stemshorn, Andrew K.

2008-07-01

High-pressure studies have been performed on heavy rare earth metals Terbium (Tb) to 155 GPa and Holmium (Ho) to 134 GPa in a diamond anvil cell at room temperature. The following crystal structure sequence was observed in both metals hcp {yields} Sm-type {yields} dhcp {yields} distorted fcc (hR-24) {yields} monoclinic (C2/m) with increasing pressure. The last transformation to a low symmetry monoclinic phase is accompanied by a volume collapse of 5 % for Tb at 51 GPa and a volume collapse of 3 % for Ho at 103 GPa. This volume collapse under high pressure is reminiscent of f-shell delocalizationmore » in light rare earth metal Cerium (Ce), Praseodymium (Pr), and heavy actinide metals Americium (Am) and Curium (Cm). The orthorhombic Pnma phase that has been reported in Am and Cm after f-shell delocalization is not observed in heavy rare earth metals under high pressures. (authors)« less

Biotransport of transuranium radionuclides in dairy animals: a data summary

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sutton, W.W.; Patzer, R.G.; Potter, G.D.

In recent years, the Environmental Monitoring Systems Laboratory at Las Vegas, Nevada (EMSL-LV) has carried out a series of studies on the biological transport of plutonium, americium, neptunium, and curium in lactating dairy cattle and goats. Ruminants in general and cattle in particular form one of the more important links in the human food chain. Milk and milk products constitute a significant portion of the human diet, especially for children. This summary consists of a compilation of detailed data from a series of previously published studies. It has been prepared to present the data from all of these studies inmore » a single source to be used by regulatory agencies in their transport modeling and hazard assessment activities. Selected source materials for the data presented in this document have been published either in the Proceedings of the Nevada Applied Ecology Group (NAEG) or as EMSL-LV publications and are listed in the References section.« less

Environmental aspects of the transuranics. A selected, annotated bibliography. Volume 9

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ensminger, J.T.; Fore, C.S.; Dailey, N.S.

This ninth published bibliography of 589 references is compiled from the Nevada Applied Ecology Information Center`s Data Base on the Environmental Aspects of the Transuranics. The data base was built to provide information support to the Nevada Applied Ecology Group (NAEG) of DOE`s Nevada Operations Office. The general scope covers environmental aspects of uranium and the transuranic elements, with emphasis on plutonium. This annotated bibliography highlights literature on plutonium 238 and 239 and americium 241 in the critical organs of man and animals. Studies on the migration of plutonium and the transplutonics through the environment are also emphasized. Supporting informationmore » on ecology of the Nevada Test Site and reviews and summarizing literature on other radionuclides have been included at the request of the NAEG. The references are arranged by subject category with leading authors appearing alphabetically within each category. Indexes are provided for author(s), geographic location, keywords, taxonomic name, title, and publication description.« less

Recovery of minor actinides from spent fuel using TPEN-immobilized gels

DOE Office of Scientific and Technical Information (OSTI.GOV)

Koyama, S.; Suto, M.; Ohbayashi, H.

2013-07-01

A series of separation experiments was performed in order to study the recovery process for minor actinides (MAs), such as americium (Am) and curium (Cm), from the actual spent fuel by using an extraction chromatographic technique. N,N,N',N'-tetrakis-(4-propenyloxy-2-pyridylmethyl) ethylenediamine (TPPEN) is an N,N,N',N'-tetrakis (2-pyridylmethyl) ethylenediamine (TPEN) analogue consisting of an incorporated pyridine ring that acts as not only a ligand but also as a site for polymerization and crosslinking of the gel. The TPPEN and N-isopropylacrylamide (NIPA) were dissolved into dimethylformamide (DMF, Wako Co., Ltd.) and a silica beads polymer, and then TTPEN was immobilized chemically in a polymer gel (somore » called TPEN-gel). Mixed oxide (MOX) fuel, which was highly irradiated up to 119 GWD/MTM in the experimental fast reactor Joyo, was used as a reference spent fuel. First, uranium (U) and plutonium (Pu) were separated from the irradiated fuel using an ion-exchange method, and then, the platinum group elements were removed by CMPO to leave a mixed solution of MAs and lanthanides. The 3 mol% TPPEN-gel was packed with as an extraction column (CV: 1 ml) and then rinsed by 0.1 M NaNO{sub 3}(pH 4.0) for pH adjustment. After washing the column by 0.01 M NaNO{sub 3} (pH 4.0), Eu was detected and the recovery rate reached 93%. The MAs were then recovered by changing the eluent to 0.01 M NaNO{sub 3} (pH 2.0), and the recovery rate of Am was 48 %. The 10 mol% TPPEN-gel was used to improve adsorption coefficient of Am and a condition of eluent temperature was changed in order to confirm the temperature swing effect on TPEN-gel for MA. More than 90% Eu was detected in the eluent after washing with 0.01 M NaNO{sub 3} (pH 3.5) at 5 Celsius degrees. Americium was backwardly detected and eluted continuously during the same condition. After removal of Eu, the eluent temperature was changed to 32 Celsius degrees, then Am was detected (pH 3.0). Finally remained Am could be stripped from TPPEN-gel by changing the pH of the eluent to 2.0. These results These results prove that the proposed recovery process for MAs is a potential candidate for future reprocessing methods based on the extraction chromatographic technique. (authors)« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hamilton, T F

Rongelap Atoll experienced close-in ''local fallout'' from nuclear weapons tests conducted by the United States (1946-58) in the northern Marshall Islands. Most of the radiation dose delivered to Rongelap Island residents during the 1950s was from radioactive elements that quickly decayed into non-radioactive elements. Since 1985, the Lawrence Livermore National Laboratory (LLNL) has continued to provide monitoring of radioactive elements from bomb testing in the terrestrial and marine environment of Rongelap Atoll. The only remaining radioactive elements of environmental importance at the atoll are radioactive cesium (cesium-137), radioactive strontium (strontium-90), different types (isotopes) of plutonium, and americium (americium-241). Cesium- 137more » and strontium-90 dissolve in seawater and are continually flushed out of the lagoon into the open ocean. The small amount of residual radioactivity from nuclear weapons tests remaining in the lagoon does not concentrate through the marine food chain. Elevated levels of cesium-137 and strontium-90 are still present in island soils and pose a potential health risk if certain types of local plants and coconut crabs are eaten in large quantities. Cesium-137 is taken up from the soil into plants and edible food products, and may end up in the body of people living on the islands and consuming local food. The presence of cesium-137 in the human body can be detected using a device called a whole body counter. A person relaxes in a chair for a few minutes while counts or measurements are taken using a detector a few inches away from the body. The whole body counting program on Rongelap Island was established in 1999 under a cooperative agreement between the Rongelap Atoll Local Government (RALG), the Republic of the Marshall Islands and the U.S. Department of Energy (DOE). Local technicians from Rongelap continue to operate the facility under supervision of scientists from LLNL. The facility permits resettlement workers living on Rongelap Island to check the amount of cesium-137 in their bodies. The amount of cesium-137 detected in resettlement workers living on Rongelap Island over the past three years is well below the level of radiation exposure considered safe by the Nuclear Claims Tribunal. Returning residents and visitors to Rongelap will also be able to receive a whole body count free of charge to check the level of cesium in their bodies. There is also a very low health risk from exposure to external sources of radiation from visiting or walking around any of the islands on the atoll.« less

Preliminary survey of separations technology applicable to the pretreatment of Hanford tank waste (1992--1993)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lawrence, W.E.; Kurath, D.E.

1994-04-01

The US Department of Energy has established the Tank Waste Remediation System (TWRS) to manage and dispose of radioactive wastes stored at the Hanford Site. Within this program are evaluations of pretreatment system alternatives through literature reviews. The information in this report was collected as part of this project at Pacific Northwest Laboratory. A preliminary survey of literature on separations recently entered into the Hanford electronic databases (1992--1993) that have the potential for pretreatment of Hanford tank waste was conducted. Separation processes that can assist in the removal of actinides (uranium, plutonium, americium), lanthanides, barium, {sup 137}Cs, {sup 90}Sr,{sup 129more » }I, {sup 63}Ni, and {sup 99}Tc were evaluated. Separation processes of interest were identified through literature searches, journal reviews, and participation in separation technology conferences. This report contains brief descriptions of the potential separation processes, the extent and/or selectivity of the separation, the experimental conditions, and observations. Information was collected on both national and international separation studies to provide a global perspective on recent research efforts.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Chumacero, E. Miguel; De Celis Alonso, B.; Martínez Hernández, M. I.

The development in semiconductor CMOS technology has enabled the creation of sensitive detectors for a wide range of ionizing radiation. These devices are suitable for photon counting and can be used in imaging and tomography X-ray diagnostics. The Medipix[1] radiation detection system is a hybrid silicon pixel chip developed for particle tracking applications in High Energy Physics. Its exceptional features (high spatial and energy resolution, embedded ultra fast readout, different operation modes, etc.) make the Medipix an attractive device for applications in medical imaging. In this work the energy characterization of a third-generation Medipix chip (Medipix3) coupled to a siliconmore » sensor is presented. We used different radiation sources (strontium 90, iron 55 and americium 241) to obtain the response curve of the hybrid detector as a function of energy. We also studied the contrast of the Medipix as a measure of pixel noise. Finally we studied the response to fluorescence X rays from different target materials (In, Pd and Cd) for the two data acquisition modes of the chip; single pixel mode and charge summing mode.« less

Independent verification of plutonium decontamination on Johnston Atoll (1992--1996)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wilson-Nichols, M.J.; Wilson, J.E.; McDowell-Boyer, L.M.

1998-05-01

The Field Command, Defense Special Weapons Agency (FCDSWA) (formerly FCDNA) contracted Oak Ridge National Laboratory (ORNL) Environmental Technology Section (ETS) to conduct an independent verification (IV) of the Johnston Atoll (JA) Plutonium Decontamination Project by an interagency agreement with the US Department of Energy in 1992. The main island is contaminated with the transuranic elements plutonium and americium, and soil decontamination activities have been ongoing since 1984. FCDSWA has selected a remedy that employs a system of sorting contaminated particles from the coral/soil matrix, allowing uncontaminated soil to be reused. The objective of IV is to evaluate the effectiveness ofmore » remedial action. The IV contractor`s task is to determine whether the remedial action contractor has effectively reduced contamination to levels within established criteria and whether the supporting documentation describing the remedial action is adequate. ORNL conducted four interrelated tasks from 1992 through 1996 to accomplish the IV mission. This document is a compilation and summary of those activities, in addition to a comprehensive review of the history of the project.« less

Extraction Selectivity of a Quaternary Alkylammonium Salt for Trivalent Actinides over Trivalent Lanthanides: Does Extractant Aggregation Play a Role?

DOE PAGES

Knight, Andrew W.; Chiarizia, Renato; Soderholm, L.

2017-05-10

In this paper, the extraction behavior of a quaternary alkylammonium salt extractant was investigated for its selectivity for trivalent actinides over trivalent lanthanides in nitrate and thiocyanate media. The selectivity was evaluated by solvent extraction experiments through radiochemical analysis of 241Am and 152/154Eu. Solvent extraction distribution and slope-analysis experiments were performed with americium(III) and europium(III) with respect to the ligand (nitrate and thiocyanate), extractant, and metal (europium only) concentrations. Further evaluation of the equilibrium expression that governs the extraction process indicated the appropriate use of the saturation method for estimation of the aggregation state of quaternary ammonium extractants in themore » organic phase. From the saturation method, we observed an average aggregation number of 5.4 ± 0.8 and 8.5 ± 0.9 monomers/aggregate for nitrate and thiocyanate, respectively. Through a side-by-side comparison of the nitrate and thiocyanate forms, we discuss the potential role of the aggregation in the increased selectivity for trivalent actinides over trivalent lanthanides in thiocyanate media.« less

Biosorption of americium-241 by immobilized Rhizopus arrihizus.

PubMed

Liao, Jiali; Yang, Yuanyou; Luo, Shunzhong; Liu, Ning; Jin, Jiannan; Zhang, Taiming; Zhao, Pengji

2004-01-01

Rhizopus arrihizus (R. arrihizus), a fungus, which in previous experiments had shown encouraging ability to remove 241Am from solutions, was immobilized by calcium alginate and other reagents. The various factors affecting 241Am biosorption by the immobilized R. arrihizus were investigated. The results showed that not only can immobilized R. arrihizus adsorb 241Am as efficiently as free R. arrihizus, but that also can be used repeatedly or continuously. The biosorption equilibrium was achieved within 2 h, and more than 94% of 241Am was removed from 241Am solutions of 1.08 MBq/l by immobilized R. arrihizu in the pH range 1-7. Temperature did not affect the adsorption on immobilized R. arrihizus in the range 15-45 degrees C. After repeated adsorption for 8 times, the immobilized R. arrihizus still adsorbed more than 97% of 241Am. At this time, the total adsorption of 241Am was more than 88.6 KBq/g, and had not yet reached saturation. Ninety-five percent of the adsorbed 241Am was desorbed by saturated EDTA solution and 98% by 2 mol/l HNO(3).

Soil and sediment sample analysis for the sequential determination of natural and anthropogenic radionuclides.

PubMed

Michel, H; Levent, D; Barci, V; Barci-Funel, G; Hurel, C

2008-02-15

A new sequential method for the determination of both natural (U, Th) and anthropogenic (Sr, Cs, Pu, Am) radionuclides has been developed for application to soil and sediment samples. The procedure was optimised using a reference sediment (IAEA-368) and reference soils (IAEA-375 and IAEA-326). Reference materials were first digested using acids (leaching), 'total' acids on hot plate, and acids in microwave in order to compare the different digestion technique. Then, the separation and purification were made by anion exchange resin and selective extraction chromatography: transuranic (TRU) and strontium (SR) resins. Natural and anthropogenic alpha radionuclides were separated by uranium and tetravalent actinide (UTEVA) resin, considering different acid elution medium. Finally, alpha and gamma semiconductor spectrometer and liquid scintillation spectrometer were used to measure radionuclide activities. The results obtained for strontium-90, cesium-137, thorium-232, uranium-238, plutonium-239+240 and americium-241 isotopes by the proposed method for the reference materials provided excellent agreement with the recommended values and good chemical recoveries. Plutonium isotopes in alpha spectrometry planchet deposits could be also analysed by ICPMS.

Predicting the response of a submillimeter bolometer to cosmic rays.

PubMed

Woodcraft, Adam L; Sudiwala, Rashmi V; Ade, Peter A R; Griffin, Matthew J; Wakui, Elley; Bhatia, Ravinder S; Lange, Andrew E; Bock, James J; Turner, Anthony D; Yun, Minhee H; Beeman, Jeffrey W

2003-09-01

Bolometers designed to detect submillimeter radiation also respond to cosmic, gamma, and x rays. Because detectors cannot be fully shielded from such energy sources, it is necessary to understand the effect of a photon or cosmic-ray particle being absorbed. The resulting signal (known as a glitch) can then be removed from raw data. We present measurements using an Americium-241 gamma radiation source to irradiate a prototype bolometer for the High Frequency Instrument in the Planck Surveyor satellite. Our measurements showed no variation in response depending on where the radiation was absorbed, demonstrating that the bolometer absorber and thermistor thermalize quickly. The bolometer has previously been fully characterized both electrically and optically. We find that using optically measured time constants underestimates the time taken for the detector to recover from a radiation absorption event. However, a full thermal model for the bolometer, with parameters taken from electrical and optical measurements, provides accurate time constants. Slight deviations from the model were seen at high energies; these can be accounted for by use of an extended model.

The efficacies of pure LICAM(C) and DTPA on the retention of plutonium-238 and americium-241 in rats after their inhalation as nitrate and intravenous injection as citrate.

PubMed

Stradling, G N; Stather, J W; Gray, S A; Moody, J C; Ellender, M; Hodgson, A; Volf, V; Taylor, D M; Wirth, P; Gaskin, P W

1989-10-01

The pure carboxylated catechoyl amide LICAM(C) and the calcium and zinc salts of diethylenetriaminepenta-acetic acid (DTPA), were tested for efficacy for removing 238Pu and 241Am from rats after inhalation of the nitrate or intravenous injection of the citrate. The results were compared with the efficacy of methylated LICAM(C) used in previous experiments. It was shown that: (1) after inhalation of 238Pu nitrate, DTPA was far superior to pure LICAM(C); (2) after intravenous injection of 238Pu citrate, the infusion of DTPA plus LICAM(C) was only marginally more effective than DTPA alone; and (3) after inhalation or intravenous injection of 238Pu plus 241Am, the efficacy of pure LICAM(C) was only marginally more effective than the methylated form and neither form was effective for the decorporation of 241Am. It was concluded that DTPA, at present, remains the chelating agent of choice for treating persons accidentally contaminated with transportable forms of Pu and Am.

a Theoretical and Experimental Investigation of 1/F Noise in the Alpha Decay Rates of AMERICIUM-241.

NASA Astrophysics Data System (ADS)

Pepper, Gary T.

New experimental methods and data analysis techniques were used to investigate the hypothesis of the existence of 1/f noise in a alpha particle emission rates for ^{241}Am. Experimental estimates of the flicker floor were found to be almost two orders of magnitude less than Handel's theoretical prediction and previous measurements. The existence of a flicker floor for ^{57}Co decay, a process for which no charged particles are emitted, indicate that instrumental instability is likely responsible for the values of the flicker floor obtained. The experimental results and the theoretical arguments presented indicate that a re-examination of Handel's theory of 1/f noise is appropriate. Methods of numerical simulation of noise processes with a 1/f^{rm n} power spectral density were developed. These were used to investigate various statistical aspects of 1/f ^{rm n} noise. The probability density function for the Allan variance was investigated in order to establish confidence limits for the observations made. The effect of using grouped (correlated) data, for evaluating the Allan variance, was also investigated.

Predicting the response of a submillimeter bolometer to cosmic rays

NASA Astrophysics Data System (ADS)

Woodcraft, Adam L.; Sudiwala, Rashmi V.; Ade, Peter A. R.; Griffin, Matthew J.; Wakui, Elley; Bhatia, Ravinder S.; Lange, Andrew E.; Bock, James J.; Turner, Anthony D.; Yun, Minhee H.; Beeman, Jeffrey W.

2003-09-01

Bolometers designed to detect submillimeter radiation also respond to cosmic, gamma, and x rays. Because detectors cannot be fully shielded from such energy sources, it is necessary to understand the effect of a photon or cosmic-ray particle being absorbed. The resulting signal (known as a glitch) can then be removed from raw data. We present measurements using an Americium-241 gamma radiation source to irradiate a prototype bolometer for the High Frequency Instrument in the Planck Surveyor satellite. Our measurements showed no variation in response depending on where the radiation was absorbed, demonstrating that the bolometer absorber and thermistor thermalize quickly. The bolometer has previously been fully characterized both electrically and optically. We find that using optically measured time constants underestimates the time taken for the detector to recover from a radiation absorption event. However, a full thermal model for the bolometer, with parameters taken from electrical and optical measurements, provides accurate time constants. Slight deviations from the model were seen at high energies; these can be accounted for by use of an extended model.

Preparation of alpha sources using magnetohydrodynamic electrodeposition for radionuclide metrology.

PubMed

Panta, Yogendra M; Farmer, Dennis E; Johnson, Paula; Cheney, Marcos A; Qian, Shizhi

2010-02-01

Expanded use of nuclear fuel as an energy resource and terrorist threats to public safety clearly require the development of new state-of-the-art technologies and improvement of safety measures to minimize the exposure of people to radiation and the accidental release of radiation into the environment. The precision in radionuclide metrology is currently limited by the source quality rather than the detector performance. Electrodeposition is a commonly used technique to prepare massless radioactive sources. Unfortunately, the radioactive sources prepared by the conventional electrodeposition method produce poor resolution in alpha spectrometric measurements. Preparing radioactive sources with better resolution and higher yield in the alpha spectrometric range by integrating magnetohydrodynamic convection with the conventional electrodeposition technique was proposed and tested by preparing mixed alpha sources containing uranium isotopes ((238)U, (234)U), plutonium ((239)Pu), and americium ((241)Am) for alpha spectrometric determination. The effects of various parameters such as magnetic flux density, deposition current and time, and pH of the sample solution on the formed massless radioactive sources were also experimentally investigated. Copyright 2009 Elsevier Inc. All rights reserved.

Report on Analyses of WAC Samples of Evaporator Overheads - 2004

DOE Office of Scientific and Technical Information (OSTI.GOV)

Oji, L

2005-03-18

In November and December of 2004, the Tank Farm submitted annual samples from 2F, 2H and 3H Evaporator Overhead streams for characterization to verify compliance with the new Effluent Treatment Facility (ETF) Waste Acceptance Criteria (WAC) and to look for organic species. With the exception of slightly high ammonia in the 2F evaporator overheads and high radiation control guide number for the 3H and 2F evaporator overhead samples, all the overheads samples were found to be in compliance with the Effluent Treatment Facility WAC. The ammonium concentration in the 2F-evaporator overhead, at 33 mg/L, was above the ETF waste watermore » collection tank (WWCT) limits of 28 mg/L. The RCG Number for the 3H and 2F evaporator samples at, respectively, 1.38E-02 and 8.24E-03 were higher than the WWCT limit of 7.69E-03. The analytical detection limits for americium-241 and radium-226 in the evaporator samples were not consistently met because of low WWCT detection limits and insufficient evaporator samples.« less

Reducing the radiation dose from inhaled americium-241 using continuously administered DTPA therapy.

PubMed

Guilmette, R A; Muggenburg, B A

1988-02-01

Accelerating the removal of a radionuclide from the body of a contaminated individual is the only available approach to decreasing the radiation dose from such exposures. In this study, continuous infusion of a chelating agent, DTPA, was given to dogs that had inhaled a moderately soluble aerosol, 241 AmO2, not only to accelerate clearance of the radionuclide from the lung but also to prevent its deposition in liver and bone. Treatment was begun with an intravenous injection of CaDTPA 1 h after exposure, and was continued for 64 days after exposure by implanting subcutaneously osmotic pumps containing ZnDTPA at 1 day after exposure. The results showed that the infusion therapy was effective in blocking the translocation of 99.5 per cent of the 241Am that would have been deposited in liver, and 98.3 per cent of the 241Am that would have been deposited in bone. This result was significantly better than the result achieved using repeated intravenous injections of DTPA, the method of treatment in current use for actinide contamination cases.

Radiochemical determination of 241Am and Pu(alpha) in environmental materials.

PubMed

Warwick, P E; Croudace, I W; Oh, J S

2001-07-15

Americium-241 and plutonium determinations will become of greater importance over the coming decades as 137Cs and 241Pu decay. The impact of 137Cs on environmental chronology has been great, but its potency is waning as it decays and diffuses. Having 241Am and Pu as unequivocal markers for the 1963 weapon fallout maximum is important for short time scale environmental work, but a fast and reliable procedure is required for their separation. The developed method described here begins by digesting samples using a lithium borate fusion although an aqua regia leachate is also effective in many instances. Isolation of the Am and Pu is then achieved using a combination of extraction chromatography and conventional anion exchange chromatography. The whole procedure has been optimized, validated, and assessed for safety. The straightforwardness of this technique permits the analysis of large numbers of samples and makes 241Am-based techniques for high-resolution sediment accumulation rate studies attractive. In addition, the technique can be employed for the sequential measurement of Pu and Am in environmental surveillance programs, potentially reducing analytical costs and turnround times.

The effect of alpha-particle and proton irradiation on the electrical and defect properties of n-GaAs

NASA Astrophysics Data System (ADS)

Goodman, S. A.; Auret, F. D.; Meyer, W. E.

1994-05-01

Radiation damage effects were studied in n-GaAs grown by organo-metallic vapour phase epitaxy (OMVPE) for a wide range of alpha-particle (2.0 MeV and 5.4 MeV) and proton (2.0 MeV) particle fluences, using an americium-241 (Am-241) radio-nuclide and a linear Van de Graaff accelerator as the particle sources. The samples were irradiated at 300 K, after fabricating palladium Schottky barrier diodes (SBDs) on the 1.2 × 10 16 cm 3 Si-doped epitaxial layers. The irradiation-induced defects are characterized using conventional deep level transient spectroscopy (DLTS). A correlation is made between the change in SBD characteristics and the quantity and type of defects introduced during irradiation. It is shown that the two parameters most susceptible to this irradiation are the reverse leakage current of the SBDs and the free carrier density of the epilayer. The introduction rate and the "signatures" of the alpha-particle and proton irradiation-induced defects are calculated and compared to those of similar defects introduced during electron irradiation.

A method for the in vivo measurement of americium-241 at long times post-exposure

DOE Office of Scientific and Technical Information (OSTI.GOV)

Neton, J.W.

1988-01-01

This study investigated an improved method for the quantitative measurement, calibration and calculation of {sup 241}Am organ burdens in humans. The techniques developed correct for cross-talk or count-rate contributions from surrounding and adjacent organ burdens and assures for the proper assignment of activity to the lungs, liver and skeleton. In order to predict the net count-rates for the measurement geometries of the skull, liver and lung, a background prediction method was developed. This method utilizes data obtained from the measurement of a group of control subjects. Based on this data, a linear prediction equation was developed for each measurement geometry.more » In order to correct for the cross-contributions among the various deposition loci, a series of surrogate human phantom structures were measured. The results of measurements of {sup 241}Am depositions in six exposure cases have been evaluated using these new techniques and have indicated that lung burden estimates could be in error by as much as 100 percent when corrections are not made for contributions to the count-rate from other organs.« less

Characteristics of radionuclide accumulation in benthic organisms and fish of the Barents and Kara Seas

DOE Office of Scientific and Technical Information (OSTI.GOV)

Matishov, G.G.; Matishov, D.G.; Rissanen, C.

1995-05-01

Artificial radionuclides play a specific role in the hydrochemical, geochemical, and hydrobiological processes that are currently occurring in the western Arctic. The existing data on radioactive contamination of different plant and animal species inhabiting the sea shelf are fragmentary. Hence, it was difficult to follow the transformation of radionuclides during their transmission along food chains, from phyto- and zoo-plankton to benthos, fish, birds, and marine mammals. In 1990-1994, the Murmansk Institute of Marine Biology organized expeditions to collect samples of residues on the sea floor and also of benthos, benthic fish, macrophytes, and other organisms inhabiting the shelf of themore » Barents and Kara Seas. These samples were tested for cesium-137, cesium-134, strontium-90, plutonium-239, plutonium-240, americium-241, and cobalt-60 in Rovaniemi (Finland) by the regional radiation administration of the Finnish Centre for Radiation and Nuclear Safety. Over 1000 tests were made. Their results provided new data on the content and distribution of these radionuclides among different components of marine ecosystems. 7 refs.« less

JOWOG 22/2 - Actinide Chemical Technology (July 9-13, 2012)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jackson, Jay M.; Lopez, Jacquelyn C.; Wayne, David M.

2012-07-05

The Plutonium Science and Manufacturing Directorate provides world-class, safe, secure, and reliable special nuclear material research, process development, technology demonstration, and manufacturing capabilities that support the nation's defense, energy, and environmental needs. We safely and efficiently process plutonium, uranium, and other actinide materials to meet national program requirements, while expanding the scientific and engineering basis of nuclear weapons-based manufacturing, and while producing the next generation of nuclear engineers and scientists. Actinide Process Chemistry (NCO-2) safely and efficiently processes plutonium and other actinide compounds to meet the nation's nuclear defense program needs. All of our processing activities are done in amore » world class and highly regulated nuclear facility. NCO-2's plutonium processing activities consist of direct oxide reduction, metal chlorination, americium extraction, and electrorefining. In addition, NCO-2 uses hydrochloric and nitric acid dissolutions for both plutonium processing and reduction of hazardous components in the waste streams. Finally, NCO-2 is a key team member in the processing of plutonium oxide from disassembled pits and the subsequent stabilization of plutonium oxide for safe and stable long-term storage.« less

Extraction Selectivity of a Quaternary Alkylammonium Salt for Trivalent Actinides over Trivalent Lanthanides: Does Extractant Aggregation Play a Role?

DOE Office of Scientific and Technical Information (OSTI.GOV)

Knight, Andrew W.; Chiarizia, Renato; Soderholm, L.

In this paper, the extraction behavior of a quaternary alkylammonium salt extractant was investigated for its selectivity for trivalent actinides over trivalent lanthanides in nitrate and thiocyanate media. The selectivity was evaluated by solvent extraction experiments through radiochemical analysis of 241Am and 152/154Eu. Solvent extraction distribution and slope-analysis experiments were performed with americium(III) and europium(III) with respect to the ligand (nitrate and thiocyanate), extractant, and metal (europium only) concentrations. Further evaluation of the equilibrium expression that governs the extraction process indicated the appropriate use of the saturation method for estimation of the aggregation state of quaternary ammonium extractants in themore » organic phase. From the saturation method, we observed an average aggregation number of 5.4 ± 0.8 and 8.5 ± 0.9 monomers/aggregate for nitrate and thiocyanate, respectively. Through a side-by-side comparison of the nitrate and thiocyanate forms, we discuss the potential role of the aggregation in the increased selectivity for trivalent actinides over trivalent lanthanides in thiocyanate media.« less

AN INTERLABORATORY COMPARISON ON THE DETERMINATION OF 241Am, 244Cm AND 252Cf IN URINE.

PubMed

Gerstmann, Udo C; Taubner, Kerstin; Hartmann, Martina

2016-09-01

An intercomparison exercise on the determination of (241)Am, (244)Cm and (252)Cf in urine was performed. Since it was designed with regard to emergency preparedness, the detection limit for each nuclide was set to 0.1 Bq per 24-h urine sample. Most of the participating laboratories were established bioassay laboratories. However, some laboratories that routinely determine (241)Am only in environmental samples were also invited in order to explore their potential for emergency bioassay analysis. Another aspect of the intercomparison was to investigate the performance of all laboratories concerning the chemical yields of the (243)Am tracer in comparison with (244)Cm and (252)Cf. In summary, both types of laboratories showed good results. There was a negative bias for the results of (244)Cm and (252)Cf, which can be explained by slightly different radiochemical behaviours of americium, curium and californium and which is in agreement with results reported in the literature. © The Author 2015. Published by Oxford University Press. All rights reserved. For Permissions, please email: journals.permissions@oup.com.

Rapid determination of actinides in asphalt samples

DOE PAGES

Maxwell, Sherrod L.; Culligan, Brian K.; Hutchison, Jay B.

2014-01-12

A new rapid method for the determination of actinides in asphalt samples has been developed that can be used in emergency response situations or for routine analysis If a radiological dispersive device (RDD), Improvised Nuclear Device (IND) or a nuclear accident such as the accident at the Fukushima Nuclear Power Plant in March, 2011 occurs, there will be an urgent need for rapid analyses of many different environmental matrices, including asphalt materials, to support dose mitigation and environmental clean up. The new method for the determination of actinides in asphalt utilizes a rapid furnace step to destroy bitumen and organicsmore » present in the asphalt and sodium hydroxide fusion to digest the remaining sample. Sample preconcentration steps are used to collect the actinides and a new stacked TRU Resin + DGA Resin column method is employed to separate the actinide isotopes in the asphalt samples. The TRU Resin plus DGA Resin separation approach, which allows sequential separation of plutonium, uranium, americium and curium isotopes in asphalt samples, can be applied to soil samples as well.« less

Sources of Radioactive Isotopes for Dirty Bombs

NASA Astrophysics Data System (ADS)

Lubenau, Joel

2004-05-01

From the security perspective, radioisotopes and radioactive sources are not created equal. Of the many radioisotopes used in industrial applications, medical treatments, and scientific research, only eight, when present in relatively large amounts in radioactive sources, pose high security risks primarily because of their prevalence and physical properties. These isotopes are americium-241, californium-252, cesium-137, cobalt-60, iridium-192, radium-226, plutonium-238, and strontium-90. Except for the naturally occurring radium-226, nuclear reactors produce the other seven in bulk commercial quantities. Half of these isotopes emit alpha radiation and would, thus, primarily pose internal threats to health; the others are mainly high-energy gamma emitters and would present both external and internal health hazards. Therefore, the response to a "dirty bomb" event depends on what type of radioisotope is chosen and how it is employed. While only a handful of major corporations produce the reactor-generated radioisotopes, they market these materials to thousands of smaller companies and users throughout the world. Improving the security of the high-risk radioactive sources will require, among other efforts, cooperation among source suppliers and regulatory agencies.

An Ab Initio Full Potential Fully Relativistic Study of the (0001) Surface of Double Hexagonal Close Packed Americium*

NASA Astrophysics Data System (ADS)

Gao, Da; Ray, Asok

2007-03-01

The electronic and geometric properties of bulk dhcp Am as well as quantum size effects in the surface energies and the work functions of the dhcp Am (0001) ultra thin films up to seven layers have been examined at nonmagnetic, ferromagnetic, and anti-ferromagnetic configurations via full-potential all-electron density-functional calculations with a mixed APW+lo/LAPW basis. The anti-ferromagnetic state including spin-orbit coupling is found to be the ground state of both bulk and the (0001) surface of dhcp Am with the 5f electrons primarily localized. Our results show that magnetic configurations and spin-orbit coupling play important roles in determining the equilibrium lattice constant, the bulk modulus as well as the localized feature of 5f electrons for dhcp Am. Quantum size effects are found to be more pronounced in work functions than in surface energies. *This work is supported by the Chemical Sciences, Geosciences and Biosciences Division, Office of Basic Energy Sciences, Office of Science, U. S. Department of Energy and the Welch Foundation, Houston, Texas.

Structural investigations of Pu{sup III} phosphate by X-ray diffraction, MAS-NMR and XANES spectroscopy

DOE Office of Scientific and Technical Information (OSTI.GOV)

Popa, Karin; Raison, Philippe E., E-mail: philippe.raison@ec.europa.eu; Martel, Laura

2015-10-15

PuPO{sub 4} was prepared by a solid state reaction method and its crystal structure at room temperature was solved by powder X-ray diffraction combined with Rietveld refinement. High resolution XANES measurements confirm the +III valence state of plutonium, in agreement with valence bond derivation. The presence of the americium (as β{sup −} decay product of plutonium) in the +III oxidation state was determined based on XANES spectroscopy. High resolution solid state {sup 31}P NMR agrees with the XANES results and the presence of a solid-solution. - Graphical abstract: A full structural analysis of PuPO{sub 4} based on Rietveld analysis ofmore » room temperature X-ray diffraction data, XANES and MAS NMR measurements was performed. - Highlights: • The crystal structure of PuPO{sub 4} monazite is solved. • In PuPO{sub 4} plutonium is strictly trivalent. • The presence of a minute amount of Am{sup III} is highlighted. • We propose PuPO{sub 4} as a potential reference material for spectroscopic and microscopic studies.« less

Overview of actinide chemistry in the WIPP

DOE Office of Scientific and Technical Information (OSTI.GOV)

Borkowski, Marian; Lucchini, Jean - Francois; Richmann, Michael K

2009-01-01

The year 2009 celebrates 10 years of safe operations at the Waste Isolation Pilot Plant (WIPP), the only nuclear waste repository designated to dispose defense-related transuranic (TRU) waste in the United States. Many elements contributed to the success of this one-of-the-kind facility. One of the most important of these is the chemistry of the actinides under WIPP repository conditions. A reliable understanding of the potential release of actinides from the site to the accessible environment is important to the WIPP performance assessment (PA). The environmental chemistry of the major actinides disposed at the WIPP continues to be investigated as partmore » of the ongoing recertification efforts of the WIPP project. This presentation provides an overview of the actinide chemistry for the WIPP repository conditions. The WIPP is a salt-based repository; therefore, the inflow of brine into the repository is minimized, due to the natural tendency of excavated salt to re-seal. Reducing anoxic conditions are expected in WIPP because of microbial activity and metal corrosion processes that consume the oxygen initially present. Should brine be introduced through an intrusion scenario, these same processes will re-establish reducing conditions. In the case of an intrusion scenario involving brine, the solubilization of actinides in brine is considered as a potential source of release to the accessible environment. The following key factors establish the concentrations of dissolved actinides under subsurface conditions: (1) Redox chemistry - The solubility of reduced actinides (III and IV oxidation states) is known to be significantly lower than the oxidized forms (V and/or VI oxidation states). In this context, the reducing conditions in the WIPP and the strong coupling of the chemistry for reduced metals and microbiological processes with actinides are important. (2) Complexation - For the anoxic, reducing and mildly basic brine systems in the WIPP, the most important inorganic complexants are expected to be carbonate/bicarbonate and hydroxide. There are also organic complexants in TRU waste with the potential to strongly influence actinide solubility. (3) Intrinsic and pseudo-actinide colloid formation - Many actinide species in their expected oxidation states tend to form colloids or strongly associate with non actinide colloids present (e.g., microbial, humic and organic). In this context, the relative importance of actinides, based on the TRU waste inventory, with respect to the potential release of actinides from the WIPP, is greater for plutonium and americium, and to less extent for uranium and thorium. The most important oxidation states for WIPP-relevant conditions are III and IV. We will present an update of the literature on WIPP-specific data, and a summary of the ongoing research related to actinide chemistry in the WIPP performed by the Los Alamos National Laboratory (LANL) Actinide Chemistry and Repository Science (ACRSP) team located in Carlsbad, NM [Reed 2007, Lucchini 2007, and Reed 2006].« less

Annual INTEC Groundwater Monitoring Report for Group 5 - Snake River Plain Aquifer (2001)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Roddy, Michael Scott

2002-02-01

This report describes the monitoring activities conducted and presents the results of groundwater sampling and water-level measurements from October 2000 to September 2001. Groundwater samples were initially collected from 41 wells from the Idaho Nuclear Technology and Engineering Center and the Central Facilities Area and analyzed for iodine-129, strontium-90, tritium, gross alpha, gross beta, technetium-99, uranium isotopes, plutonium isotopes, neptunium-237, americium-241, gamma spectrometry, and mercury. Samples from 41 wells were collected in April and May 2001. Additional sampling was conducted in August 2001 and included the two CFA production wells, the CFA point of compliance for the production wells, onemore » well that was previously sampled and five additional monitoring wells. Iodine-129 and strontium-90 were the only analytes above their respective maximum contaminant levels. Iodine-129 was detected just above its maximum contaminant level of 1 pCi/L at two of the Central Facilities Area landfill wells. Iodine-129 was detected in the CFA production wells at 0.35±0.083 pCi/L in CFA-1, but was below detectable activity in CFA-2. Strontium-90 was above its maximum contaminant level of 8 pCi/L in several wells near the Idaho Nuclear Technology and Engineering Center but was below its maximum contaminant level in the downgradient wells at the Central Facilities Area landfills. Sr-90 was not detected in the CFA production wells. Gross beta results generally mirrored the results for strontium-90 and technetium-99. Plutonium isotopes and neptunium-237 were not detected. Uranium-233/234 and uranium-238 isotopes were detected in all samples. Concentrations of background and site wells were similar and are within background limits for total uranium determined by the USGS, suggesting that the concentrations are background. Uranium-235/236 was detected in 11 samples, but all the detected concentrations were similar and near the minimum detectable activity. Americium-241 was detected at three locations near the minimum detectable activity of approximately 0.07 pCi/L. The gamma spectrometry results detected cesium-137 in three samples, potassium-40 at eight locations, and radium-226 at one location. Mercury was below its maximum contaminant level of 2 µg/L in all samples. Gamma spectrometry results for the CFA production wells did not detect any analytes. Water-level measurements were taken from wells in the Idaho Nuclear Technology and Engineering Center, Central Facilities Area, and the area south of Central Facilities Area to evaluate groundwater flow directions. Water-level measurements indicated groundwater flow to the south-southwest from the Idaho Nuclear Technology and Engineering Center.« less

New Synthetic Methods and Structure-Property Relationships in Neptunium, Plutonium, and Americium Borates. Final report

DOE Office of Scientific and Technical Information (OSTI.GOV)

Albrecht-Schmitt, Thomas Edward

The past three years of support by the Heavy Elements Chemistry Program have been highly productive in terms of advanced degrees awarded, currently supported graduate students, peer-reviewed publications, and presentations made at universities, national laboratories, and at international conferences. Ph.D. degrees were granted to Shuao Wang and Juan Diwu, who both went on to post-doctoral appointments at the Glenn T. Seaborg Center at Lawrence Berkeley National Laboratory with Jeff Long and Ken Raymond, respectively. Pius Adelani completed his Ph.D. with me and is now a post-doc with Peter C. Burns. Andrea Alsobrook finished her Ph.D. and is now a post-docmore » at Savannah River with Dave Hobbs. Anna Nelson completed her Ph.D. and is now a post-doc with Rod Ewing at the University of Michigan. As can be gleaned from this list, students supported by the Heavy Elements Chemistry grant have remained interested in actinide science after leaving my program. This follows in line with previous graduates in this program such as Richard E. Sykora, who did his post-doctoral work at Oak Ridge National Laboratory with R. G. Haire, and Amanda C. Bean, who is a staff scientist at Los Alamos National Laboratory, and Philip M. Almond and Thomas C. Shehee, who are both staff scientists at Savannah River National Laboratory, Gengbang Jin who is a staff scientist at Argonne National Lab, and Travis Bray who has been a post-doc at both LBNL and ANL. Clearly this program is serving as a pipe-line for students to enter into careers in the national laboratories. About half of my students depart the DOE complex for academia or industry. My undergraduate researchers also remain active in actinide chemistry after leaving my group. Dan Wells was a productive undergraduate of mine, and went on to pursue a Ph.D. on uranium and neptunium chalcogenides with Jim Ibers at Northwestern. After earning his Ph.D., he went directly into the nuclear industry.« less

An Investigation of Aggregation in Synergistic Solvent Extraction Systems

NASA Astrophysics Data System (ADS)

Jackson, Andy Steven

With an increasing focus on anthropogenic climate change, nuclear reactors present an attractive option for base load power generation with regard to air pollution and carbon emissions, especially when compared with traditional fossil fuel based options. However, used nuclear fuel (UNF) is highly radiotoxic and contains minor actinides (americium and curium) which remain more radiotoxic than natural uranium ore for hundreds of thousands of years, presenting a challenge for long-term storage . Advanced nuclear fuel recycling can reduce this required storage time to thousands of years by removing the highly radiotoxic minor actinides. Many advanced separation schemes have been proposed to achieve this separation but none have been implemented to date. A key feature among many proposed schemes is the use of more than one extraction reagent in a single extraction phase, which can lead to the phenomenon known as "synergism" in which the extraction efficiency for a combination of the reagents is greater than that of the individual extractants alone. This feature is not well understood for many systems and a comprehensive picture of the mechanism behind synergism does not exist. There are several proposed mechanisms for synergism though none have been used to model multiple extraction systems. This work examines several proposed advanced extractant combinations which exhibit synergism: 2-bromodecanoic acid (BDA) with 2,2':6',2"-terpyridine (TERPY), tri-n-butylphosphine oxide (TPBO) with 2-thenoyltrifluoro acetone (HTTA), and dinonylnaphthalene sulfonic acid (HDNNS) with 5,8-diethyl-7-hydroxy-dodecan-6-oxime (LIX). We examine two proposed synergistic mechanisms involving and attempt to verify the ability of these mechanisms to predict the extraction behavior of the chosen systems. These are a reverse micellar catalyzed extraction model and a mixed complex formation model. Neither was able to effectively predict the synergistic behavior of the systems. We further examine these systems for the presence of large reverse micellar aggregates and thermodynamic signatures of aggregation. Behaviors differed widely from system to system, suggesting the possibility of more than one mechanism being responsible for similar observed extraction trends.

Laser decontamination of the radioactive lightning rods

NASA Astrophysics Data System (ADS)

Potiens, A. J.; Dellamano, J. C.; Vicente, R.; Raele, M. P.; Wetter, N. U.; Landulfo, E.

2014-02-01

Between 1970 and 1980 Brazil experienced a significant market for radioactive lightning rods (RLR). The device consists of an air terminal with one or more sources of americium-241 attached to it. The sources were used to ionize the air around them and to increase the attraction of atmospheric discharges. Because of their ineffectiveness, the nuclear regulatory authority in Brazil suspended the license for manufacturing, commerce and installation of RLR in 1989, and determined that the replaced RLR were to be collected to a centralized radioactive waste management facility for treatment. The first step for RLR treatment is to remove the radioactive sources. Though they can be easily removed, some contaminations are found all over the remaining metal scrap that must decontaminated for release, otherwise it must be treated as radioactive waste. Decontamination using various chemicals has proven to be inefficient and generates large amounts of secondary wastes. This work shows the preliminary results of the decontamination of 241Am-contaminated metal scrap generated in the treatment of radioactive lightning rods applying laser ablation. A Nd:YAG nanoseconds laser was used with 300 mJ energy leaving only a small amount of secondary waste to be treated.

Selected radionuclides important to low-level radioactive waste management

DOE Office of Scientific and Technical Information (OSTI.GOV)

NONE

1996-11-01

The purpose of this document is to provide information to state representatives and developers of low level radioactive waste (LLW) management facilities about the radiological, chemical, and physical characteristics of selected radionuclides and their behavior in the environment. Extensive surveys of available literature provided information for this report. Certain radionuclides may contribute significantly to the dose estimated during a radiological performance assessment analysis of an LLW disposal facility. Among these are the radionuclides listed in Title 10 of the Code of Federal Regulations Part 61.55, Tables 1 and 2 (including alpha emitting transuranics with half-lives greater than 5 years). Thismore » report discusses these radionuclides and other radionuclides that may be significant during a radiological performance assessment analysis of an LLW disposal facility. This report not only includes essential information on each radionuclide, but also incorporates waste and disposal information on the radionuclide, and behavior of the radionuclide in the environment and in the human body. Radionuclides addressed in this document include technetium-99, carbon-14, iodine-129, tritium, cesium-137, strontium-90, nickel-59, plutonium-241, nickel-63, niobium-94, cobalt-60, curium -42, americium-241, uranium-238, and neptunium-237.« less

Composition of Radioactive Aerosols in the Shelter Construction of the Chernobyl Nuclear Power Plant in 2000-2015

NASA Astrophysics Data System (ADS)

Ogorodnikov, B. I.

2018-06-01

The results of the physicochemical studies of radioactive aerosols inside and outside the Shelter construction at the Arch construction stage of the Chernobyl Nuclear Power Plant (ChNPP) in 2000-2015 were presented. The dominant isotopes were shown to be cesium, strontium, americium, plutonium, and uranium. They are carried by disperse particles of 2-7 μm. In subreactor rooms, in particular, 012/7, the composition of aerosols is affected by the erosion of the fuel-containing mass formed in 1986. Submicron cesium carrier aerosols appear as a result of evaporation and condensation during fires and welding works. Radiocesium is a well-soluble component of aerosols, while plutonium isotopes are not readily soluble components. In several rooms, the contents of radon, thoron, and their daughter products exceeded the permissible values. In April-June 2011, the intake of radionuclides from the accident at the Japanese Fukushima-1 NPP, which had AMAD of 0.5 μm, was detected and tracked using Petryanov multilayer filters. The productivity of filtration units under the dusty conditions in the exclusion zone of ChNPP and in fogs and haze was investigated. Hydrophilic prefilters with 7-10 μm fibers were recommended.

Evaluation of historical and analytical data on the TAN TSF-07 Disposal Pond

DOE Office of Scientific and Technical Information (OSTI.GOV)

Medina, S.M.

1993-07-01

The Technical Support Facility (TSF)-07 Disposal Pond, located at Test Area North at the Idaho National Engineering Laboratory, has been identified as part of Operable Unit 1-06 under the Comprehensive Environmental Response, Compensation, and Liability Act. The Environmental Restoration and Waste Management Department is conducting an evaluation of existing site characterization data for the TSF-07 Disposal Pond Track 1 investigation. The results from the site characterization data will be used to determine whether the operable unit will undergo a Track 2 investigation, an interim action, a remedial investigation/feasibility study, or result in a no-action decision. This report summarizes activities relevantmore » to wastewaters discharged to the pond and characterization efforts conducted from 1982 through 1991. Plan view and vertical distribution maps of the significant contaminants contained in the pond are included. From this evaluation it was determined that cobalt-60, cesium-137, americium-241, mercury, chromium, and thallium are significant contaminants for soils. This report also evaluates the migration tendencies of the significant contaminants into the perched water zone under the pond and the surrounding terrain to support the investigation.« less

Concealed nuclear material identification via combined fast-neutron/γ-ray computed tomography (FNGCT): a Monte Carlo study

NASA Astrophysics Data System (ADS)

Licata, M.; Joyce, M. J.

2018-02-01

The potential of a combined and simultaneous fast-neutron/γ-ray computed tomography technique using Monte Carlo simulations is described. This technique is applied on the basis of a hypothetical tomography system comprising an isotopic radiation source (americium-beryllium) and a number (13) of organic scintillation detectors for the production and detection of both fast neutrons and γ rays, respectively. Via a combination of γ-ray and fast neutron tomography the potential is demonstrated to discern nuclear materials, such as compounds comprising plutonium and uranium, from substances that are used widely for neutron moderation and shielding. This discrimination is achieved on the basis of the difference in the attenuation characteristics of these substances. Discrimination of a variety of nuclear material compounds from shielding/moderating substances (the latter comprising lead or polyethylene for example) is shown to be challenging when using either γ-ray or neutron tomography in isolation of one another. Much-improved contrast is obtained for a combination of these tomographic modalities. This method has potential applications for in-situ, non-destructive assessments in nuclear security, safeguards, waste management and related requirements in the nuclear industry.

Cerium neodymium oxide solid solution synthesis as a potential analogue for substoichiometric AmO2 for radioisotope power systems

NASA Astrophysics Data System (ADS)

Watkinson, E. J.; Ambrosi, R. M.; Williams, H. R.; Sarsfield, M. J.; Stephenson, K.; Weston, D. P.; Marsh, N.; Haidon, C.

2017-04-01

The European Space Agency (ESA) is sponsoring a research programme on the development of americium oxides for radioisotope generators and heater units. Cubic AmO2-(x/2) with an O/Am ratio between 1.65 and 1.75 is a potentially suitable compound for pellet sintering. C-type (Ia-3) Ce1-xNdxO2-(x/2) oxides with 0.5 < x < 0.7 could be used as a surrogate for some Ia-3 AmO2-(x/2). A new Ce1-xNdxO2-(x/2) production process has been investigated where a nominally selected x value of 0.6 was targeted: Ce and Nd nitrates and oxalic acid were added drop-wise into a vessel, where they continuously reacted to create oxalate precipitates. The effect of temperature (25 °C, 60 °C) of the reactants (mixed at 250 revolutions per minute) on oxalate particle shape and size were investigated. Oxalates were calcined at 900 °C to produce oxide particles. Oxalate particle properties were characterised as these are expected to influence oxides particle properties and fuel pellet sintering.

Defect annealing of alpha-particle irradiated n-GaAs

NASA Astrophysics Data System (ADS)

Goodman, S. A.; Auret, F. D.; Myburg, G.

1994-09-01

The annealing behaviour of irradiation induced defects in n-type GaAs irradiated at 300 K with 5.4 MeV alpha-particles from an americium-241 (Am-241) radio nuclide have been investigated. The annealing kinetics are presented for the alpha-particle induced defects Eα1 Eα5 detected in Organo-Metallic Vapor Phase Epitaxially (OMVPE) grown n-GaAs doped with silicon to 1.2×1016 cm-3, these kinetics are compared to those obtained for similar defects (E1 E5) detected after electron irradiation. While defects Pα1 and Pα2 were detected after removal of the electron defects Eα4 and Eα5, respectively, a new defect labelled Pα0, located 0.152 eV below the conduction band, was introduced by annealing. The thermal behaviour and trap characteristics of these three defects (Pα0 Pα2) are presented. In an attempt to further characterise defects Pα0 and Pα1 a preiliminary study investigating the emission rate field dependence of these defects was conducted, it was observed that defect Pα0 exhibited a fairly strong field dependence while Pα1 exhibited a much weaker dependence.

Medical and health physics management of a plutonium wound

DOE Office of Scientific and Technical Information (OSTI.GOV)

Carbaugh, E.H.; Decker, W.A.; Swint, M.J.

1988-04-01

A puncture wound contaminated with plutonium and americium has provided an excellent case study for dealing with internal contamination. This case provides an opportunity to examine the effectiveness of diagnostic techniques, therapeutic techniques, dose assessment practices, and case management philosophy. The wound deposited 48 kBq of transuranic alpha activity in the right index finger. Minor surgery reduced the long-term wound burden to about 5.4 kBq. Chelation therapy with DTPA lasted 17 months and resulted in urinary excretion of about 7 kBq of the deposited activity. Therapy appears to have been effective in limiting early uptake and internal doses from thismore » wound. However, the possibility of slow future uptake from the wound exists. Thus, estimating long-term uptake and dose is difficult. In vivo measurements indicate that residual wound contamination is essentially constant. Within three weeks of the injury, an initial measurable liver burden was reduced by chelation therapy to below detectable limits, and no subsequent build-up has been observed. However, there is indication of a gradually increasing skeleton burden. The axillary lymph nodes have shown relatively constant, detectable activity. 8 refs., 3 figs.« less

Study on the PGNAA measurement of heavy metals in aqueous solution by the Monte Carlo-Library Least-Squares (MCLLS) approach.

PubMed

Zhang, Yan; Jia, WenBao; Gardner, Robin; Shan, Qing; Hei, Daqian

2018-02-01

In the present work, a prompt gamma neutron activation analysis (PGNAA) setup, which consists of a 300mCi 241 Americium-Beryllium (Am-Be) neutron source and a 4 × 4-in. Bismuth germanium oxide (BGO) detector, was developed for heavy metal detection in aqueous solutions. A series of standard samples with analytical purity were prepared by dissolving heavy metals in deionized water. Quantitative spectrum analysis was performed by the Monte Carlo-Least-Squares (MCLLS) approach to measure the standard samples. The detector response functions of 4 × 4-in. BGO detector were generated by using the CEARDRF code. The element libraries were simulated in silico by the CEARCPG code, which was developed by Dr. Gardner. The simulation results presented were in very good agreement with the experimental results. The correlation coefficients were very close to 1 when the fitted spectrum was compared with the experimental spectrum. By applying the MCLLS approach, the relative deviation of the measurement accuracy was less than 2.27% for Ni, Mn, and Cu and up to 69.33% for Pb. Copyright © 2017 Elsevier Ltd. All rights reserved.

Streamlined Approach for Environmental Restoration (SAFER) Plan for Corrective Action Unit 415: Project 57 No. 1 Plutonium Dispersion (NTTR), Nevada, Revision 0

DOE Office of Scientific and Technical Information (OSTI.GOV)

Matthews, Patrick; Burmeister, Mark

2014-04-01

This Streamlined Approach for Environmental Restoration (SAFER) Plan addresses the actions needed to achieve closure for Corrective Action Unit (CAU) 415, Project 57 No. 1 Plutonium Dispersion (NTTR). CAU 415 is located on Range 4808A of the Nevada Test and Training Range (NTTR) and consists of one corrective action site: NAFR-23-02, Pu Contaminated Soil. The CAU 415 site consists of the atmospheric release of radiological contaminants to surface soil from the Project 57 safety experiment conducted in 1957. The safety experiment released plutonium (Pu), uranium (U), and americium (Am) to the surface soil over an area of approximately 1.9 squaremore » miles. This area is currently fenced and posted as a radiological contamination area. Vehicles and debris contaminated by the experiment were subsequently buried in a disposal trench within the surface-contaminated, fenced area and are assumed to have released radiological contamination to subsurface soils. Potential source materials in the form of pole-mounted electrical transformers were also identified at the site and will be removed as part of closure activities.« less

Final Technical Report

DOE Office of Scientific and Technical Information (OSTI.GOV)

Dr. Asok K. Ray

2012-05-22

During the past decades, considerable theoretical efforts have been devoted to studying the electronic and geometric structures and related properties of surfaces. Such efforts are particularly important for systems like the actinides for which experimental work is relatively difficult to perform due to material problems and toxicity. The actinides are characterized by a gradual filling of the 5f-electron shell with the degree of localization increasing with the atomic number Z along the last series of the periodic table. The open shell of the 5f electrons determines the atomic, molecular, and solid state properties of the actinide elements and their compoundsmore » and understanding the quantum mechanics of the 5f electrons is the defining issue in the chemistry and physics of actinide elements. These elements are also characterized by the increasing prominence of relativistic effects and their studies can, in fact, help us understand the role of relativity throughout the periodic table. However, the electronic and geometric structures of the actinides, specifically the trans-uranium actinides and the roles of the 5f electrons in chemical bonding are still not well understood. This is crucial not only for our understanding of the actinides but also for the fact that the actinides constitute 'the missing link' between the d transition elements and the lanthanides. The 5f orbitals have properties intermediate between those of localized 4f and delocalized 3d orbitals. Thus, a proper understanding of the actinides will help us understand the behavior of the lanthanides and transition metals as well. In fact, there is an urgent need for continued extensive and detailed theoretical research in this area to provide significant and deep understandings of the electronic and geometric structures of the actinides. In this work, we have performed electronic structure studies for plutonium (Pu), americium (Am), and curium (Cm) surfaces, and molecular adsorptions on Pu and Am surfaces. In particular, the region at the boundary of Pu and Am, is widely believed to be the crossover region between d-like itinerant and f-like localized behavior The eventual goal is a complete understanding of the surface chemistry and physics processes of all actinide surfaces, defining the chemistry and physics of such heavy elements. Among the actinides, plutonium, with five 5f electrons in the solid state, is arguably the most complex, fascinating, and enigmatic element known to mankind and has attracted extraordinary scientific and technological interests because of its unique properties, generating a significant body of research in diverse areas, including superconductivity. Pu has, at least, six stable allotropes between room temperature and melting at atmospheric pressure, indicating that the valence electrons can hybridize into a number of complex bonding arrangements. Central and critical questions relate to the electronic structure, localization of the 5f electrons and the magnetism of Pu. For the light-actinides, from Th to Pu, the 5f electrons are believed to be delocalized, hybridizing with the 6d and 7s electrons. For the heavier actinides, Am and beyond, the 5f electrons are localized with the 5f orbitals progressively lower in energy relative to the 6d configuration. Hence, Pu is in a position where the 5f electronic behavior changes from itinerant to localized. As far as magnetism is concerned, a majority of the theoretical calculations continues to claim the existence of magnetism while almost all the experimental results do not find any support for such claims. The second element of interest to us, namely americium, occupies a central position in the actinide series with respect to the involvement of 5f electrons in metallic bonding. It is widely believed that the 5f electrons in Am are localized and that Am undergoes a series of crystallographic phase changes with pressure. Fully-relativistic all electron surface studies of the different phases of Am, initially for the dhcp and the fcc surfaces, can and have provided us with valuable information about chemical bonding in Am and the transitions from f-electron delocalization to f-electron localization in trans-uranium compounds. In particular, a comparative study of the electronic structures of the Pu and Am surfaces using the techniques of all-electron modern density functional theory and beyond can provide significant information about the role of 5f electrons in bond formation as also the localization of the 5f electrons, matters of considerable controversies. The change from metallic 5f bonding into local-moment nonbonding configurations that takes place between Pu and Am is rather unique in the periodic table and is at the very heart of our understanding of electronic structure. We believe that, considering the narrow bandwidth of surface states, any transition from itinerant to localized behavior first takes place at the actinide surfaces with possible reconstructions.« less

Progress in Modeling Pu Properties and Aging - ESC Review, March 19-23, 2001

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wolfer, W G; Caturla, M; Kubota, A

2001-03-29

An important component of the Pu aging programs both here at LLNL and at LANL is the development of models for the aging processes. These models will, in the foreseeable future, be validated with more and more data from different experiments, and eventually enable us to predict the lifetime of pits. The processes of aging from within the material are mainly caused by the radioactive decay of Pu, and this produces three drivers for changes in properties: (1) Radiation damage in the form of displacements, of defects, of dislocations, and voids. (2) Helium will aggregate in the form of bubblesmore » and cavities. (3) Uranium, Americium, and Neptunium will change the chemical composition and perhaps the phase stability. All the three drivers act synergistically, no doubt. But it is useful to approach the complexity of Pu aging with the strategy of ''first divide, conquer, and then unify''. In this spirit, we have divided the program into three major task areas with individual subtasks to be conquered by various researchers. The subtasks and staffing has changed somewhat from last year, and this is indicated on the viewgraph by underlines. Undoubtedly, it will change in the future, but the objectives of the major tasks and of the entire project will not change until the mission as stated at the beginning will have been accomplished. As you see from the third task, there is a strong emphasis on providing theoretical and computational support for critical, fundamental experiments. Before reviewing the progress made last year for the various tasks, let me briefly state what the physical properties are that we monitor for signs of aging. Prominent is the change in density and microstructure, and its effects on strength and EOS. You will hear little if anything at all about the latter two properties, but work is in progress on these issues, and the review committee will hear about it at the next review. For this review, I want to concentrate on dimensional changes and the underlying changes in microstructure. Once we understand the changes in the microstructure, we can perhaps predict its influence on strength and EOS. It forms the basis for the predictive capability that we want to develop.« less

LITERATURE REVIEW ON THE SORPTION OF PLUTONIUM, URANIUM, NEPTUNIUM, AMERICIUM AND TECHNETIUM TO CORROSION PRODUCTS ON WASTE TANK LINERS

DOE Office of Scientific and Technical Information (OSTI.GOV)

Li, D.; Kaplan, D.

2012-02-29

The Savannah River Site (SRS) has conducted performance assessment (PA) calculations to determine the risk associated with closing liquid waste tanks. The PA estimates the risk associated with a number of scenarios, making various assumptions. Throughout all of these scenarios, it is assumed that the carbon-steel tank liners holding the liquid waste do not sorb the radionuclides. Tank liners have been shown to form corrosion products, such as Fe-oxyhydroxides (Wiersma and Subramanian 2002). Many corrosion products, including Fe-oxyhydroxides, at the high pH values of tank effluent, take on a very strong negative charge. Given that many radionuclides may have netmore » positive charges, either as free ions or complexed species, it is expected that many radionuclides will sorb to corrosion products associated with tank liners. The objective of this report was to conduct a literature review to investigate whether Pu, U, Np, Am and Tc would sorb to corrosion products on tank liners after they were filled with reducing grout (cementitious material containing slag to promote reducing conditions). The approach was to evaluate radionuclides sorption literature with iron oxyhydroxide phases, such as hematite ({alpha}-Fe{sub 2}O{sub 3}), magnetite (Fe{sub 3}O{sub 4}), goethite ({alpha}-FeOOH) and ferrihydrite (Fe{sub 2}O{sub 3} {center_dot} 0.5H{sub 2}O). The primary interest was the sorption behavior under tank closure conditions where the tanks will be filled with reducing cementitious materials. Because there were no laboratory studies conducted using site specific experimental conditions, (e.g., high pH and HLW tank aqueous and solid phase chemical conditions), it was necessary to extend the literature review to lower pH studies and noncementitious conditions. Consequently, this report relied on existing lower pH trends, existing geochemical modeling, and experimental spectroscopic evidence conducted at lower pH levels. The scope did not include evaluating the appropriateness of K{sub d} values for the Fe-oxyhydroxides, but instead to evaluate whether it is a conservative assumption to exclude this sorption process of radionuclides onto tank liner corrosion products in the PA model. This may identify another source for PA conservatism since the modeling did not consider any sorption by the tank liner.« less

A method of discriminating transuranic radionuclides from radon progeny using low-resolution alpha spectroscopy and curve-fitting techniques.

PubMed

Konzen, Kevin; Brey, Richard

2012-05-01

²²²Rn (radon) and ²²⁰Rn (thoron) progeny are known to interfere with determining the presence of long-lived transuranic radionuclides, such as plutonium and americium, and require from several hours up to several days for conclusive results. Methods are proposed that should expedite the analysis of air samples for determining the amount of transuranic radionuclides present using low-resolution alpha spectroscopy systems available from typical alpha continuous air monitors (CAMs) with multi-channel analyzer (MCA) capabilities. An alpha spectra simulation program was developed in Microsoft Excel visual basic that employed the use of Monte Carlo numerical methods and serial-decay differential equations that resembled actual spectra. Transuranic radionuclides were able to be quantified with statistical certainty by applying peak fitting equations using the method of least squares. Initial favorable results were achieved when samples containing radon progeny were decayed 15 to 30 min, and samples containing both radon and thoron progeny were decayed at least 60 min. The effort indicates that timely decisions can be made when determining transuranic activity using available alpha CAMs with alpha spectroscopy capabilities for counting retrospective air samples if accompanied by analyses that consider the characteristics of serial decay.

Investigation of Workplace-like Calibration Fields via a Deuterium-Tritium (D-T) Neutron Generator.

PubMed

Mozhayev, Andrey V; Piper, Roman K; Rathbone, Bruce A; McDonald, Joseph C

2017-04-01

Radiation survey meters and personal dosimeters are typically calibrated in reference neutron fields based on conventional radionuclide sources, such as americium-beryllium (Am-Be) or californium-252 (Cf), either unmodified or heavy-water moderated. However, these calibration neutron fields differ significantly from the workplace fields in which most of these survey meters and dosimeters are being used. Although some detectors are designed to yield an approximately dose-equivalent response over a particular neutron energy range, the response of other detectors is highly dependent upon neutron energy. This, in turn, can result in significant over- or underestimation of the intensity of neutron radiation and/or personal dose equivalent determined in the work environment. The use of simulated workplace neutron calibration fields that more closely match those present at the workplace could improve the accuracy of worker, and workplace, neutron dose assessment. This work provides an overview of the neutron fields found around nuclear power reactors and interim spent fuel storage installations based on available data. The feasibility of producing workplace-like calibration fields in an existing calibration facility has been investigated via Monte Carlo simulations. Several moderating assembly configurations, paired with a neutron generator using the deuterium tritium (D-T) fusion reaction, were explored.

A Novel Technique for Raman Analysis of Highly Radioactive Samples Using Any Standard Micro-Raman Spectrometer

PubMed Central

Colle, Jean-Yves; Naji, Mohamed; Sierig, Mark; Manara, Dario

2017-01-01

A novel approach for the Raman measurement of nuclear materials is reported in this paper. It consists of the enclosure of the radioactive sample in a tight capsule that isolates the material from the atmosphere. The capsule can optionally be filled with a chosen gas pressurized up to 20 bars. The micro-Raman measurement is performed through an optical-grade quartz window. This technique permits accurate Raman measurements with no need for the spectrometer to be enclosed in an alpha-tight containment. It therefore allows the use of all options of the Raman spectrometer, like multi-wavelength laser excitation, different polarizations, and single or triple spectrometer modes. Some examples of measurements are shown and discussed. First, some spectral features of a highly radioactive americium oxide sample (AmO2) are presented. Then, we report the Raman spectra of neptunium oxide (NpO2) samples, the interpretation of which is greatly improved by employing three different excitation wavelengths, 17O doping, and a triple mode configuration to measure the anti-stokes Raman lines. This last feature also allows the estimation of the sample surface temperature. Finally, data that were measured on a sample from Chernobyl lava, where phases are identified by Raman mapping, are shown. PMID:28448046

DOE Office of Scientific and Technical Information (OSTI.GOV)

None, None

Operations of Sandia National Laboratories, Nevada (SNL/NV) at the Tonopah Test Range (TTR) resulted in no planned point radiological releases during 1996. Other releases from SNL/NV included diffuse transuranic sources consisting of the three Clean Slate sites. Air emissions from these sources result from wind resuspension of near-surface transuranic contaminated soil particulates. The total area of contamination has been estimated to exceed 20 million square meters. Soil contamination was documented in an aerial survey program in 1977 (EG&G 1979). Surface contamination levels were generally found to be below 400 pCi/g of combined plutonium-238, plutonium-239, plutonium-240, and americium-241 (i.e., transuranic) activity.more » Hot spot areas contain up to 43,000 pCi/g of transuranic activity. Recent measurements confirm the presence of significant levels of transuranic activity in the surface soil. An annual diffuse source term of 0.39 Ci of transuranic material was calculated for the cumulative release from all three Clean Slate sites. A maximally exposed individual dose of 1.1 mrem/yr at the TTR airport area was estimated based on the 1996 diffuse source release amounts and site-specific meteorological data. A population dose of 0.86 person-rem/yr was calculated for the local residents. Both dose values were attributable to inhalation of transuranic contaminated dust.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Klumpp, John Allan; Bertelli, Luiz; Waters, Tom L.

For radionuclides such as plutonium and americium, detection of removable activity in the nose (i.e., nasal swab measurements) are frequently used to determine whether follow-up bioassay measurements are warranted following a potential intake. For this paper, the authors analyzed 429 nasal swab measurements taken following incidents or suspicious circumstances (such as an air monitor alarming) at Los Alamos National Laboratory (LANL) for which the dose was later evaluated using in vitro bioassay. Nasal swab measurements were found to be very poor predictors of dose and should not be used as such in the field. However, nasal swab measurements can bemore » indicative of whether a reliably detectable committed effective dose (CED) occurred. About 14% of nasal swab measurements between 1.25 and 16.7 Bq corresponded to CEDs greater than 1 mSv, so in general, positive nasal swabs always indicate that follow-up bioassay should be performed (positive nasal swabs less than 1.25 Bq are considered separately). This probability increased significantly for nasal swabs greater than 16.7 Bq. Only about 3% of nasal swabs with no detectable activity (NDA) corresponded to reliably detectable CEDs. As a result, a nasal swab with NDA is therefore necessary, but not sufficient, to negate the need for a follow-up bioassay if it was collected following other workplace indicators of a potential intake.« less

An aerial radiological survey of Maralinga and EMU, South Australia

DOE Office of Scientific and Technical Information (OSTI.GOV)

Tipton, W J; Berry, H A; Fritzsche, A E

An aerial radiological survey was conducted over the former British nuclear test ranges at Maralinga and Emu in South Australia from May through July 1987. The survey covered an area of approximately 1,550 square kilometers which included the nine major trial sites, where a nuclear yield occurred, and all the minor trial sites, where physics experiments were conducted. Flight lines were flown at an altitude of 30 meters with line spacings of 50, 100, and 200 meters depending on the area and whether man-made contamination was present. Results of the aerial survey were processed for americium-241 (used to determine plutoniummore » contamination), cesium-137, cobalt-60, and uranium-238. The aerial survey also detected the presence of europium-152, a soil activation product, in the immediate vicinity of the major trial ground zeros. Ground measurements were also made at approximately 120 locations using a high-resolution germanium detector to provide supplemental data for the aerial survey. This survey was conducted as part of a series of studies being conducted over a two to three-year timeframe to obtain information from which options and associated costs can be formulated about the decontamination and possible rehabilitation of the former nuclear test sites.« less

Radiochemical Procedures Used at Iaea-Ilmr Monaco for Measuring Artificial Radionuclides Resulting from the Chernobyl Accident

NASA Astrophysics Data System (ADS)

Ballestra, S.; Gastaud, J.; Lopez, J. J.

The Chernobyl accident which occurred on 26 April 1986 resulted in relatively high levels of radioactive fallout over the major part of Europe. Air filter and precipitation samples enabled us to follow the contamination from the accident. In addition contamination was also monitored in selected environmental samples such as seaweeds, sea water, sediment, soil, suspended matter and biological material from the Mediterranean. All samples were counted on Ge(Li) or Ge(HP) detectors to determine the type and quantity of gamma emitting radionuclides and plutonium, americium and curium isotopes were separated and measured using radiochemical techniques and alpha counting. Increased atmospheric radioactivity from the Chernobyl accident was first detected by observing increased activity levels on air filters taken on April 30, 1986, with maximum activities occurring during 1-3 May. Most of the radionuclides initially measured were short-lived fission products. Cs-137 was one of the predominant isotope in the fallout debris and its deposition at Monaco due to Chernobyl was estimated to be around 1400 Bq m-2, which represents 25-40% of the integrated fallout at this latitude. The deposition of Pu-239+240 was much smaller and was estimated to be around 10 mBq m-2 or only 0.1% of the total deposition from nuclear weapon testing.

Chemical Characterization of an Envelope B/D Sample from Hanford Tank 241-AZ-102

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hay, M.S.

2000-08-23

A sample from Hanford waste tank 241-AZ-102 was received at the Savannah River Technology Center (SRTC) and chemically characterized. The sample containing supernate and a small amount of sludge solids was analyzed as-received. The filtered supernatant liquid, the total dried solids of the sample, and the washed insoluble solids obtained from filtration of the sample were analyzed. A mass balance calculation of the three fractions of the sample analyzed indicate the analytical results appear relatively self-consistent for major components of the sample. However, some inconsistency was observed between results were more than one method of determination was employed and formore » species present in low concentrations. The actinides isotopes, plutonium, americium, and curium, present analytical challenges due to the low concentration of these species and the potential for introduction of small amounts of contamination during sampling handling resulting in large uncertainties. A direct comparison to previous analyses of material from tank 241-AZ-102 showed good agreement with the filtered supernatant liquid. However, the comparison of solids data showed poor agreement. The poor agreement shown between the current results for the solids samples and previous analyses most likely results from the uncertainties associated with obtaining small solids samples from a large non-homogenized waste tank.« less

Gastrointestinal absorption of americium-241 by orally exposed swine: comparison of experimental results with predictions of metabolic models.

PubMed

Eisele, G R; Bernard, S R; Nestor, C W

1987-10-01

Two groups of 11-week-old swine (40 miniature and 40 domestic swine) received a single oral administration of 1.9 X 10(8) Bq (5.2 mCi) of 241Am citrate, and groups of eight animals, four of each type, were killed and sampled at 1, 2, 4, 8, 16, 24, 48, 72, and 96 h and 30 days later. Uptake and excretion patterns of the radioactivity appeared to occur in three phases: rapid uptake, rapid excretion, and then a slower excretion. All animals were systematically dissected, and the eviscerated carcasses were autoclaved for separation of bone and muscle. The predominant site of deposition was bone, and autoclaving had little effect on releasing 241Am from either bone or muscle. The maximum fractional gastrointestinal absorption of 1.1 X 10(-3) occurred 8 h after radionuclide administration. The tissue distribution data suggest partitions of 50, 20, and 30%, for bone, liver, and other soft tissues, respectively. Two metabolic models were evaluated: a modified Mewhinney-Griffith model and the ICRP 30 model to compare the biological data with model predictions. All models underestimated the actual early time data, but the fits to the experimental results were better at later times.

XPS studies of UO 2 oxidation by alpha radiolysis of water at 100°C

NASA Astrophysics Data System (ADS)

Sunder, S.; Boyer, G. D.; Miller, N. H.

1990-12-01

The effect of alpha radiolysis of water on the oxidation and dissolution of UO 2 was studied at 100°C as a function of alpha-field strength and water chemistry using X-ray photoelectron spectroscopy. In N 2-purged solutions the oxidation of UO 2 increases with the strength of the alpha flux; an alpha flux greater than or equal to that from a 250-μ Ci americium-241 source leads to oxidation of UO 2 beyond the UO 2.33 (U 3O 7) stage, and an alpha flux equal to that from a 5-μ Ci source does not result in UO 2 oxidation beyond the UO 2.33 stage. The presence of dissolved H 2 in water, at a concentration ≥ 1.6 × 10 -4moldm-3, reduces the oxidation and dissolution of UO 2 due to alpha radiolysis at temperatures ≥ 100° C. It is concluded that the radiolysis of groundwater at ~ 100°C, due to the alpha flux associated with used CANDU fuel, is unlikely to make a significant contribution to its oxidative dissolution in the geological disposal vault planned in the Canadian Nuclear Fuel Waste Management Program. CANada Deuterium Uranium. Registered trademark.

The NITON{reg_sign} XL-800 Series Multi-Element Spectrum Analyzer (Alloy Analyzer). Innovative Technology Summary Report

DOE Office of Scientific and Technical Information (OSTI.GOV)

None

2000-04-01

The NITON{reg_sign} 800 series analyzer is a hand-held, battery operated unit that measures 8-in x 3-in x 2-in and weighs 2.5 pounds. The analyzer uses x-ray fluorescence spectrum analysis to identify and quantify elements in metal and then compares the readings to a built-in library to determine a metal's alloy. The library contains 300 elements and alloys, and can be customized to identify other elements and alloys (depending on the sources in the instrument). The basic unit utilizes a Cadmium-109 source, but each analyzer unit can hold up to two sources. These sources include Iron-55 and Americium-241. Pushing a safetymore » button located on the side of the unit and placing it against a surface opens the shutter window. Within seconds the unit beeps, and displays the results. The analyzer stores up to 1,000 data sets, including sample identification codes using a barcode reader. The data is easily downloaded to a conventional computer when sampling has been completed. Batteries are good for 8-hrs and charge in less than 2 hours and it can be carried, shipped, or transported without exterior labeling, conforming to 49 CFR 143.421.« less

High temperature heat capacity of (U, Am)O2±x

NASA Astrophysics Data System (ADS)

Epifano, E.; Beneš, O.; Vălu, O. S.; Zappey, J.; Lebreton, F.; Martin, P. M.; Guéneau, C.; Konings, R. J. M.

2017-10-01

Mixed uranium and americium dioxides (U, Am)O2±x are candidates as possible transmutation targets for generation IV reactors. In this work, the enthalpy increments of this solid solution were measured in the 470-1750 K temperature range by drop calorimetry for Am/(Am + U) ratios equal to 0.32, 0.39, 0.49, 0.58 and 0.68. Then, the heat capacity functions were obtained by derivation of the enthalpy data. The results of this work were compared to the heat capacity and enthalpy functions reported in the literature for the UO2 [1] and AmO2 [2] binary oxides and for the U0.9Am0.1O2±x, U0.8Am0.2O2±x mixed oxides [3]. From the obtained trend, it was found out that an excess contribution to the enthalpy increment appears for T > 1100 K in the compositions with Am/(Am + U)≥0.4 and a possible explanation attributing this effect to oxygen hypostoichiometry is provided. Finally, to verify the hypothesis, thermodynamic computations based on the CALPHAD method were performed for AmO2-x under air and the results confirmed that the source of the excess contribution is the formation of oxygen vacancies.

Insight into the Am-O Phase Equilibria: A Thermodynamic Study Coupling High-Temperature XRD and CALPHAD Modeling.

PubMed

Epifano, Enrica; Guéneau, Christine; Belin, Renaud C; Vauchy, Romain; Lebreton, Florent; Richaud, Jean-Christophe; Joly, Alexis; Valot, Christophe; Martin, Philippe M

2017-07-03

In the frame of minor actinide transmutation, americium can be diluted in UO 2 and (U, Pu)O 2 fuels burned in fast neutron reactors. The first mandatory step to foresee the influence of Am on the in-reactor behavior of transmutation targets or fuel is to have fundamental knowledge of the Am-O binary system and, in particular, of the AmO 2-x phase. In this study, we coupled HT-XRD (high-temperature X-ray diffraction) experiments with CALPHAD thermodynamic modeling to provide new insights into the structural properties and phase equilibria in the AmO 2-x -AmO 1.61+x -Am 2 O 3 domain. Because of this approach, we were able for the first time to assess the relationships between temperature, lattice parameter, and hypostoichiometry for fcc AmO 2-x . We showed the presence of a hyperstoichiometric existence domain for the bcc AmO 1.61+x phase and the absence of a miscibility gap in the fcc AmO 2-x phase, contrary to previous representations of the phase diagram. Finally, with the new experimental data, a new CALPHAD thermodynamic model of the Am-O system was developed, and an improved version of the phase diagram is presented.

SEE induced in SRAM operating in a superconducting electron linear accelerator environment

NASA Astrophysics Data System (ADS)

Makowski, D.; Mukherjee, Bhaskar; Grecki, M.; Simrock, Stefan

2005-02-01

Strong fields of bremsstrahlung photons and photoneutrons are produced during the operation of high-energy electron linacs. Therefore, a mixed gamma and neutron radiation field dominates the accelerators environment. The gamma radiation induced Total Ionizing Dose (TID) effect manifests the long-term deterioration of the electronic devices operating in accelerator environment. On the other hand, the neutron radiation is responsible for Single Event Effects (SEE) and may cause a temporal loss of functionality of electronic systems. This phenomenon is known as Single Event Upset (SEU). The neutron dose (KERMA) was used to scale the neutron induced SEU in the SRAM chips. Hence, in order to estimate the neutron KERMA conversion factor for Silicon (Si), dedicated calibration experiments using an Americium-Beryllium (241Am/Be) neutron standard source was carried out. Single Event Upset (SEU) influences the short-term operation of SRAM compared to the gamma induced TID effect. We are at present investigating the feasibility of an SRAM based real-time beam-loss monitor for high-energy accelerators utilizing the SEU caused by fast neutrons. This paper highlights the effects of gamma and neutron radiations on Static Random Access Memory (SRAM), placed at selected locations near the Superconducting Linear Accelerator driving the Vacuum UV Free Electron Laser (VUVFEL) of DESY.

Timing and Pulse Shape Discrimination Comparison Against Legacy TDC & QDC and the JLab F250 FADC

NASA Astrophysics Data System (ADS)

Milkeris-Zellar, Tyler; Sawatzky, Brad

2017-09-01

The F250 Flash Analog to Digital Convertor (FADC) is a relatively new module used in Data Acquisition Systems (DAQ) at Jefferson Lab. The FADC will replace or supplement older DAQ modules like Time to Digital Converters (TDCs) and Charge Analog to Digital Converters (QDCs). The TDC has a certain known timing resolution and the QDC can integrate a pulse's charge, a feature which can also be used for particle identification between photons and neutrons using pulse shape discrimination (PSD). The focus of this project is developing a test stand to study timing and PSD performance of legacy modules TDC and QDC, and the new F250 FADC. A cosmic telescope was used to extract timing resolution from the TDC and FADC. Through PSD with the QDC and FADC, using a liquid scintillator, we plan to identify photons and neutrons from an americium-beryllium (AmBe) source. Through PSD, we found that the FADC allows for flexible data analysis compared to the QDC. The results indicate that the TDC provides a more accurate measurement of timing resolution than the FADC. This improvement allows for a clear distinction of what module to use when wanting precision of measurement in a DAQ for a cosmic ray telescope. NSF.

Method of photon spectral analysis

DOEpatents

Gehrke, Robert J.; Putnam, Marie H.; Killian, E. Wayne; Helmer, Richard G.; Kynaston, Ronnie L.; Goodwin, Scott G.; Johnson, Larry O.

1993-01-01

A spectroscopic method to rapidly measure the presence of plutonium in soils, filters, smears, and glass waste forms by measuring the uranium L-shell x-ray emissions associated with the decay of plutonium. In addition, the technique can simultaneously acquire spectra of samples and automatically analyze them for the amount of americium and .gamma.-ray emitting activation and fission products present. The samples are counted with a large area, thin-window, n-type germanium spectrometer which is equally efficient for the detection of low-energy x-rays (10-2000 keV), as well as high-energy .gamma. rays (>1 MeV). A 8192- or 16,384 channel analyzer is used to acquire the entire photon spectrum at one time. A dual-energy, time-tagged pulser, that is injected into the test input of the preamplifier to monitor the energy scale, and detector resolution. The L x-ray portion of each spectrum is analyzed by a linear-least-squares spectral fitting technique. The .gamma.-ray portion of each spectrum is analyzed by a standard Ge .gamma.-ray analysis program. This method can be applied to any analysis involving x- and .gamma.-ray analysis in one spectrum and is especially useful when interferences in the x-ray region can be identified from the .gamma.-ray analysis and accommodated during the x-ray analysis.

Method of photon spectral analysis

DOEpatents

Gehrke, R.J.; Putnam, M.H.; Killian, E.W.; Helmer, R.G.; Kynaston, R.L.; Goodwin, S.G.; Johnson, L.O.

1993-04-27

A spectroscopic method to rapidly measure the presence of plutonium in soils, filters, smears, and glass waste forms by measuring the uranium L-shell x-ray emissions associated with the decay of plutonium. In addition, the technique can simultaneously acquire spectra of samples and automatically analyze them for the amount of americium and [gamma]-ray emitting activation and fission products present. The samples are counted with a large area, thin-window, n-type germanium spectrometer which is equally efficient for the detection of low-energy x-rays (10-2,000 keV), as well as high-energy [gamma] rays (>1 MeV). A 8,192- or 16,384 channel analyzer is used to acquire the entire photon spectrum at one time. A dual-energy, time-tagged pulser, that is injected into the test input of the preamplifier to monitor the energy scale, and detector resolution. The L x-ray portion of each spectrum is analyzed by a linear-least-squares spectral fitting technique. The [gamma]-ray portion of each spectrum is analyzed by a standard Ge [gamma]-ray analysis program. This method can be applied to any analysis involving x- and [gamma]-ray analysis in one spectrum and is especially useful when interferences in the x-ray region can be identified from the [gamma]-ray analysis and accommodated during the x-ray analysis.

Bituminization of radioactive wastes: safety studies

DOE Office of Scientific and Technical Information (OSTI.GOV)

Arod, J.

1982-01-01

The bitumen embedding of low- and medium-level radioactive wastes has reached the industrial stage. Bituminization plants are operating satisfactorily in France and throughout the world. However, bituminization presents certain risks due to the nature of bitumens themselves. These risks must be taken into account. This paper specifies those risks and presents the results of leachability tests performed in accordance with the International Atomic Energy Agency proposed standard on coated concentrates, on chemical coprecipitation sludges with and without addition of heavy solvents such as TBP and TLA, and on ion exchange resins. The results show that the leaching rates in demineralizedmore » water are on the order of 10/sup -6/ to 10/sup -8/ for cesium 137, 10/sup -5/ to 10/sup -7/ for strontium-90, 10/sup -5/ to 10/sup -6/ for ruthemium-106, 10/sup -5/ to 10/sup -6/ for cobalt-60, 10/sup -5/ to 10/sup -6/ for total gamma activity, and 10/sup -5/ to 10/sup -8/ for the plutonium-238, the plutonium-239, and the americium 241 alpha emitters. Even if this conditioning is not perfect, the storage of low- and medium-level radioactive wastes is made possible with adequate safety and at a reasonable cost.« less

United States transuranium and uranium registries - 25 years of growth, research, and service. Annual report, April 1992--September 1993

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kathren, R.L.; Harwick, L.A.; Toohey, R.E.

The Registries originated in 1968 as the National Plutonium Registry with the name changed to the United States Transuranium Registry the following year to reflect a broader concern with the heavier actinides as well. Initially, the scientific effort of the USTR was directed towards study of the distribution and dose of plutonium and americium in occupationally exposed persons, and to assessment of the effects of exposure to the transuranium elements on health. This latter role was reassessed during the 1970`s when it was recognized that the biased cohort of the USTR was inappropriate for epidemiologic analysis. In 1978, the administrativelymore » separate but parallel United States Uranium Registry was created to carry out similar work among persons exposed to uranium and its decay products. A seven member scientific advisory committee provided guidance and scientific oversight. In 1992, the two Registries were administratively combined and transferred from the purview of a Department of Energy contractor to Washington State University under the provisions of a grant. Scientific results for the first twenty-five years of the Registries are summarized, including the 1985 publication of the analysis of the first whole body donor. Current scientific work in progress is summarized along with administrative activities for the period.« less

Mixed Metal Phosphonate- Phosphate Resins for Separation of Lanthanides from Actinides

DOE Office of Scientific and Technical Information (OSTI.GOV)

Clearfield, Abraham

As indicated in the previous annual report the goals of this project are to develop procedures for efficient separation of lanthanides from actinides and curium from americium. These processes are required for the nuclear fuel cycle to minimize the waste and recover the valuable actinides. The basis for our study is that we have prepared a group of compounds that are porous and favor the uptake of ions with charges 3+ and 4+ over ions of lesser charge. The general formula for these materials is M(O 3PC 6H 4PO 3) 1-x/2(APO 4)x·nH 2O: where M=Zr 4+, Sn 4+, A=H, Na,more » or K and X=O, 0.5, 0.8, 1.0, 1.33 and 1.61-3. One of our tasks is to determine which members of this group of compounds are effective in carrying out the required separations. A difficulty in obtaining this required information is that the compounds are amorphous. That is they are not crystalline, therefore we need to resort to synchrotron data to obtain structural data which will be presented in detail. This information will be provided as a separate section.« less

Impact of the uranium (VI) speciation in mineralised urines on its extraction by calix[6]arene bearing hydroxamic groups used in chromatography columns.

PubMed

Baghdadi, S; Bouvier-Capely, C; Ritt, A; Peroux, A; Fevrier, L; Rebiere, F; Agarande, M; Cote, G

2015-11-01

Actinides determination in urine samples is part of the analyses performed to monitor internal contamination in case of an accident or a terrorist attack involving nuclear matter. Mineralisation is the first step of any of these analyses. It aims at reducing the sample volume and at destroying all organic compounds present. The mineralisation protocol is usually based on a wet ashing step, followed by actinides co-precipitation and a furnace ashing step, before redissolution and the quantification of the actinides by the appropriate techniques. Amongst the existing methods to perform the actinides co-precipitation, alkali-earth (typically calcium) precipitation is widely used. In the present work, the extraction of uranium(VI), plutonium(IV) and americium(III) from the redissolution solutions (called "mineralised urines") on calix[6]arene columns bearing hydroxamic groups was investigated as such an extraction is a necessary step before their determination by ICP-MS or alpha spectrometry. Difficulties were encountered in the transfer of uranium(VI) from raw to mineralised urines, with yield of transfer ranging between 0% and 85%, compared to about 90% for Pu and Am, depending on the starting raw urines. To understand the origin of such a difficulty, the speciation of uranium (VI) in mineralised urines was investigated by computer simulation using the MEDUSA software and the associated HYDRA database, compiled with recently published data. These calculations showed that the presence of phosphates in the "mineralised urines" leads to the formation of strong uranyl-phosphate complexes (such as UO2HPO4) which compete with the uranium (VI) extraction by the calix[6]arene bearing hydroxamic groups. The extraction constant of uranium (VI) by calix[6]arene bearing hydroxamic groups was determined in a 0.04 mol L(-1) sodium nitrate solution (logK=4.86±0.03) and implemented in an extraction model taking into account the speciation in the aqueous phase. This model allowed to simulate satisfactorily the experimental uranium extraction data and to support the preliminary conclusions about the role of the phosphates present in mineralised urines. These calculations also showed that the phosphate/calcium ratio is a key parameter as far as the efficiency of the uranium (VI) extraction by the calix[6]arene columns is concerned. It predicted that the addition of CaCl2 in mineralised urines would release uranium (VI) from phosphates by forming calcium (II)-phosphate complexes and thus facilitate the uranium (VI) extraction on calix[6]arene columns. These predictions were confirmed experimentally as the addition of 0.1 mol L(-1) CaCl2 to a mineralised urine containing naturally a high concentration of phosphate (typically 0.04 mol L(-1)) significantly increased the percentage of uranium (VI) extraction on the calix[6]arene columns. Copyright © 2015 Elsevier B.V. All rights reserved.

Effects on radionuclide concentrations by cement/ground-water interactions in support of performance assessment of low-level radioactive waste disposal facilities

DOE Office of Scientific and Technical Information (OSTI.GOV)

Krupka, K.M.; Serne, R.J.

The US Nuclear Regulatory Commission is developing a technical position document that provides guidance regarding the performance assessment of low-level radioactive waste disposal facilities. This guidance considers the effects that the chemistry of the vault disposal system may have on radionuclide release. The geochemistry of pore waters buffered by cementitious materials in the disposal system will be different from the local ground water. Therefore, the cement-buffered environment needs to be considered within the source term calculations if credit is taken for solubility limits and/or sorption of dissolved radionuclides within disposal units. A literature review was conducted on methods to modelmore » pore-water compositions resulting from reactions with cement, experimental studies of cement/water systems, natural analogue studies of cement and concrete, and radionuclide solubilities experimentally determined in cement pore waters. Based on this review, geochemical modeling was used to calculate maximum concentrations for americium, neptunium, nickel, plutonium, radium, strontium, thorium, and uranium for pore-water compositions buffered by cement and local ground-water. Another literature review was completed on radionuclide sorption behavior onto fresh cement/concrete where the pore water pH will be greater than or equal 10. Based on this review, a database was developed of preferred minimum distribution coefficient values for these radionuclides in cement/concrete environments.« less

Interpretation of nasal swab measurements following suspected releases of actinide aerosols

DOE PAGES

Klumpp, John Allan; Bertelli, Luiz; Waters, Tom L.

2017-05-01

For radionuclides such as plutonium and americium, detection of removable activity in the nose (i.e., nasal swab measurements) are frequently used to determine whether follow-up bioassay measurements are warranted following a potential intake. For this paper, the authors analyzed 429 nasal swab measurements taken following incidents or suspicious circumstances (such as an air monitor alarming) at Los Alamos National Laboratory (LANL) for which the dose was later evaluated using in vitro bioassay. Nasal swab measurements were found to be very poor predictors of dose and should not be used as such in the field. However, nasal swab measurements can bemore » indicative of whether a reliably detectable committed effective dose (CED) occurred. About 14% of nasal swab measurements between 1.25 and 16.7 Bq corresponded to CEDs greater than 1 mSv, so in general, positive nasal swabs always indicate that follow-up bioassay should be performed (positive nasal swabs less than 1.25 Bq are considered separately). This probability increased significantly for nasal swabs greater than 16.7 Bq. Only about 3% of nasal swabs with no detectable activity (NDA) corresponded to reliably detectable CEDs. As a result, a nasal swab with NDA is therefore necessary, but not sufficient, to negate the need for a follow-up bioassay if it was collected following other workplace indicators of a potential intake.« less

Photoneutron Flux Measurement via Neutron Activation Analysis in a Radiotherapy Bunker with an 18 MV Linear Accelerator

NASA Astrophysics Data System (ADS)

Çeçen, Yiğit; Gülümser, Tuğçe; Yazgan, Çağrı; Dapo, Haris; Üstün, Mahmut; Boztosun, Ismail

2017-09-01

In cancer treatment, high energy X-rays are used which are produced by linear accelerators (LINACs). If the energy of these beams is over 8 MeV, photonuclear reactions occur between the bremsstrahlung photons and the metallic parts of the LINAC. As a result of these interactions, neutrons are also produced as secondary radiation products (γ,n) which are called photoneutrons. The study aims to map the photoneutron flux distribution within the LINAC bunker via neutron activation analysis (NAA) using indium-cadmium foils. Irradiations made at different gantry angles (0°, 90°, 180° and 270°) with a total of 91 positions in the Philips SLI-25 linear accelerator treatment room and location-based distribution of thermal neutron flux was obtained. Gamma spectrum analysis was carried out with high purity germanium (HPGe) detector. Results of the analysis showed that the maximum neutron flux in the room occurred at just above of the LINAC head (1.2x105 neutrons/cm2.s) which is compatible with an americium-beryllium (Am-Be) neutron source. There was a 90% decrease of flux at the walls and at the start of the maze with respect to the maximum neutron flux. And, just in front of the LINAC door, inside the room, neutron flux was measured less than 1% of the maximum.

Annual report of the United States transuranium and uranium registries, October 1, 1988--September 30, 1989

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kathren, R.L.; Swint, M.J.; Dietert, S.E.

1990-04-01

This report summarizes the primary scientific activities of the United States Transuranium and Uranium Registries for the period October 1, 1988 through September 30, 1989. The Registries are parallel human tissue research programs devoted to the study of the actinide elements in man. The emphasis of the Transuranium Registry was directed toward evaluation of six whole body donations. In the five cases whose exposure was through inhalation, approximately half of the total body content of Pu-239 + 240 and a third of the Am-241 was found in the respiratory tract, suggesting that these nuclides are more avidly retained than predictedmore » by the current model of the International Commission on Radiological Protection. A significant fraction of these nuclides is found in soft tissues other than liver, and an uptake fraction of 0.2 is proposed for muscle, with a residence half-time of 10 years. Studies of these and routine autopsy cases indicate that more than 90% of the total respiratory tract plutonium or americium is in the lungs, with the remainder in the lymph nodes, and that a greater fraction is found in the lungs of smokers relative to the lymph nodes. Primary activities of the Uranium Registry centered around the acquisition of a whole body donation from a woman who had received an injection of colloidal thorium dioxide some 38 years prior to death.« less

Plutonium-239 + 240 and Americium-241 in soils east of Rocky Flats, Colorado

DOE Office of Scientific and Technical Information (OSTI.GOV)

Litaor, M.I.; Barth, G.R.; Molzer, P.C.

1994-11-01

Soils east of the Rocky Flats (RF) near Golden, CO, were contaminated with Pu-239 + 240 and Am-241 as a result of past waste-storage practices. The physiocochemical parameters that govern the actinides distribution in the soil are poorly understood. Twenty-six soil pits at various distances and directions from a contaminated site at RF were excavated, sampled, and analyzed for actinide activities as well as selected physical, chemical, and mineralogical attributes. Plutonium-239+240 and Am-241 activities in the soils ranged form 164 280 Bq/kg to 0.0037 Bq/kg, decreasing with distance from the source. More than 90% of the Pu-239 + 240 andmore » Am-241 activities were confined to the upper 12 cm of the soil, regardless of the soil characteristics, or distance and direction from the source. Evidence of preferential transport in macropores formed along decayed root channels was observed in four soil pits and had translocated Pu-239 + 240 to a depth of 90 cm. This transport mechanism increased by a factor of 30 the level of Pu-239 + 240 activity at this depth. Earthworm activity is probably important in the redistribution of actinides in the upper 40 cm of many of the soils investigated. Planning of future remedial activities at RF should consider the findings of this contaminant-transport study. 34 refs., 5 figs., 2 tabs.« less

Vertical migration of plutonium-239 + -240, americium-241 and caesium-137 fallout in a forest soil under spruce.

PubMed

Bunzl, K; Kracke, W; Schimmack, W

1992-03-01

The vertical activity distributions of fallout 238Pu, 239+240Pu, 241Am, 134Cs and 137Cs in a forest soil (Hapludult) were determined at several locations in a spruce stand separately according to their origin (global fallout or Chernobyl fallout). To determine the rate of migration of these radionuclides in each soil horizon, the observed depth profiles of the radionuclides were evaluated with a compartment model. In the top organic horizons (LOf1 and Of2), the migration rates for all radionuclides from both sources were above 0.5 cm per year. In the Oh horizon the migration rates observed for global fallout Pu, Am and Cs were similar (0.2-0.4 cm per year). Compared with Pu, however, the mobility of Am is slightly, but statistically significantly, enhanced. The highest rate in this layer was found for Chernobyl-derived radiocaesium (2 cm per year). In the layers of the mineral horizon (depth 0-2, 2-5 and 5-10 cm) the observed migration rates were very similar for global fallout Pu (0.08-0.7 cm per year) and Am (0.1-2 cm per year). In comparison, the migration rate of global fallout radiocaesium was about half in each layer. The highest rate was observed again for Chernobyl-derived radiocaesium (0.5-3 cm per year).

Amchitka Island, Alaska, special sampling project 1997

DOE Office of Scientific and Technical Information (OSTI.GOV)

U.S. Department of Energy, Nevada Operations Office

2000-06-28

This 1997 special sampling project represents a special radiobiological sampling effort to augment the 1996 Long-Term Hydrological Monitoring Program (LTHMP) for Amchitka Island in Alaska. Lying in the western portion of the Aleutian Islands arc, near the International Date Line, Amchitka Island is one of the southernmost islands of the Rat Island Chain. Between 1965 and 1971, the U.S. Atomic Energy Commission conducted three underground nuclear tests on Amchitka Island. In 1996, Greenpeace collected biota samples and speculated that several long-lived, man-made radionuclides detected (i.e., americium-241, plutonium-239 and -240, beryllium-7, and cesium-137) leaked into the surface environment from underground cavitiesmore » created during the testing. The nuclides of interest are detected at extremely low concentrations throughout the environment. The objectives of this special sampling project were to scientifically refute the Greenpeace conclusions that the underground cavities were leaking contaminants to the surface. This was achieved by first confirming the presence of these radionuclides in the Amchitka Island surface environment and, second, if the radionuclides were present, determining if the source is the underground cavity or worldwide fallout. This special sampling and analysis determined that the only nonfallout-related radionuclide detected was a low level of tritium from the Long Shot test, which had been previously documented. The tritium contamination is monitored and continues a decreasing trend due to radioactive decay and dilution.« less

Maternal transfer of anthropogenic radionuclides to eggs in a small shark.

PubMed

Jeffree, Ross A; Oberhansli, Francois; Teyssie, Jean-Louis; Fowler, Scott W

2015-09-01

Maternal transfer of radionuclides to progeny is one of the least known sources of contamination in marine biota and more information is needed to assess its radiological significance. A radiotracer study on spotted dogfish, Scyliorhinus canicula, evaluated the hypothesis that four anthropogenic radionuclides (Cobalt-60, Zinc-65, Americium-241 and Cesium-134) could be maternally transferred to eggs and each of their major components during maternal ingestion of radiolabelled food. The linear regressions between cumulative radioactivity that had been maternally ingested and the level in subsequently laid eggs were used to derive maternal-to-egg transfer factors (mTFs). These maternal transfers varied over an order of magnitude and were ranked (134)Cs > (65)Zn > (60)Co > (241)Am. This ranking was the same as their relative assimilation efficiencies in radiolabelled food consumed by adults. Among these four radionuclides the potential radiological exposure of embryos is accentuated for (65)Zn and (134)Cs due to their predominant transfer to egg yolk where they are available for subsequent absorption by the embryo as it develops prior to hatching from the egg capsule. Thus, for cartilaginous fish like shark, the potential radioecological consequences of a pulsed release of these radionuclides into the marine environment may extend beyond the temporal duration of the release. Copyright © 2015 Elsevier Ltd. All rights reserved.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bürger, Stefan; Riciputi, Lee R; Bostick, Debra A

A ThermoFisher 'Triton' multi-collector thermal ionization mass spectrometer (MC-TIMS) was evaluated for trace and ultra-trace level isotoperatioanalysis of actinides (uranium, plutonium, and americium), fission products and geolocators (strontium, cesium, and neodymium). Total efficiencies (atoms loaded to ions detected) of up to 0.5-2% for U, Pu, and Am, and 1-30% for Sr, Cs, and Nd can be reported employing resin bead load techniques onto flat ribbon Re filaments or resin beads loaded into a millimeter-sized cavity drilled into a Re rod. This results in detection limits of <0.1 fg (10{sup 4} atoms to 10{sup 5} atoms) for {sup 239-242+244}Pu, {sup 233+236}U,more » {sup 241-243}Am, {sup 89,90}Sr, and {sup 134,135,137}Cs, and {le} 1 pg for natural Nd isotopes (limited by the chemical processing blank) using a secondary electron multiplier (SEM) or multiple-ion counters (MICs). Relative standard deviations (RSD) as small as 0.1% and abundance sensitivities of 1 x 10{sup 6} or better using a SEM are reported here. Precisions of RSD {approx} 0.01-0.001% using a multi-collector Faraday cup array can be achieved at sub-nanogram concentrations for strontium and neodymium and are suitable to gain crucial geolocation information. The analytical protocols reported herein are of particular value for nuclear forensic and nuclear safeguard applications.« less

Savannah River Site Spent Nuclear Fuel Management Final Environmental Impact Statement

DOE Office of Scientific and Technical Information (OSTI.GOV)

N /A

The proposed DOE action considered in this environmental impact statement (EIS) is to implement appropriate processes for the safe and efficient management of spent nuclear fuel and targets at the Savannah River Site (SRS) in Aiken County, South Carolina, including placing these materials in forms suitable for ultimate disposition. Options to treat, package, and store this material are discussed. The material included in this EIS consists of approximately 68 metric tons heavy metal (MTHM) of spent nuclear fuel 20 MTHM of aluminum-based spent nuclear fuel at SRS, as much as 28 MTHM of aluminum-clad spent nuclear fuel from foreign andmore » domestic research reactors to be shipped to SRS through 2035, and 20 MTHM of stainless-steel or zirconium-clad spent nuclear fuel and some Americium/Curium Targets stored at SRS. Alternatives considered in this EIS encompass a range of new packaging, new processing, and conventional processing technologies, as well as the No Action Alternative. A preferred alternative is identified in which DOE would prepare about 97% by volume (about 60% by mass) of the aluminum-based fuel for disposition using a melt and dilute treatment process. The remaining 3% by volume (about 40% by mass) would be managed using chemical separation. Impacts are assessed primarily in the areas of water resources, air resources, public and worker health, waste management, socioeconomic, and cumulative impacts.« less

A flowsheet concept for an Am/Ln separation based on Am{sup VI} solvent extraction

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mincher, B.J.; Law, J.D.

2013-07-01

The separation of Am from the lanthanides and curium is a key step in proposed advanced fuel cycle scenarios. The partitioning and transmutation of Am is desirable to minimize the long-term radiotoxicity of material interred in a future high-level waste repository. However, a separation amenable to process scale-up remains elusive. Higher oxidation states of americium have recently been used to demonstrate solvent extraction-based separations using conventional fuel cycle ligands. Here, the successful partitioning of Am{sup VI} from the bulk of lanthanides and curium using diamyl-amyl-phosphonate (DAAP) extraction is reported. Due to the instability of Am{sup VI} in the organic phasemore » it was readily selectively stripped to a new acidic aqueous phase to provide separation from co-extracted Ce{sup IV}. The use of NaBiO{sub 3} as an oxidant to separate Am from the lanthanides and Cm by solvent extraction has been successfully demonstrated on the bench scale. Based on these results, flowsheet concepts can be designed that result in 96 % Am recovery in the presence of a few percent of the remaining Cm and the lanthanides in two extraction contacts. Preliminary results also indicate that the DAAP extractant is robust toward γ- irradiation under realistic conditions of acidity and dissolved oxygen concentration.« less

Durability test on irradiated rock-like oxide fuels

NASA Astrophysics Data System (ADS)

Kuramoto, K.; Nitani, N.; Yamashita, T.

2003-06-01

For a profitable use of Pu, Japan Atomic Energy Research Institute has been promoting researches for once-through type fuels. The strategy consists of stable rock-like oxide fuel fabrication in conventional fuel facilities followed by almost complete Pu burning in LWR and disposal of chemically stable spent fuel without further processing. Because leach rates of hazardous nuclides, such as TRU and β-emitters, that have long half-lives, are very important for the evaluation of geological safety, leaching tests in deionized water at 363 K were performed with reference to the MCC-1 method. Five irradiated fuel pellets, a single phase fuel of a yttria-stabilized zirconia (YSZ) containing UO 2 (U-YSZ), two fuels of U-YSZ particle dispersed in MgAl 2O 4 (SPI) or Al 2O 3 (COR) matrix, two homogeneous-blended fuels of U-YSZ and SPI or COR powders, were submitted to the tests. Stainless steel containers with Au coating and ethylene propylene diene monomer were used as leaching vessels and packing, respectively. The evaluated normalized leach rates of Zr, U and Pu were obviously lower than those of the other important elements and nuclides. Americium, Np and especially Y showed unexpectedly high evaluated normalized leach rates. The volatile elements, Cs and I, showed enhanced leaching within particle-dispersed type fuels because of crack formation around the particle.

LWR First Recycle of TRU with Thorium Oxide for Transmutation and Cross Sections

DOE Office of Scientific and Technical Information (OSTI.GOV)

Andrea Alfonsi; Gilles Youinou; Sonat Sen

2013-02-01

Thorium has been considered as an option to uranium-based fuel, based on considerations of resource utilization (thorium is approximately three times more plentiful than uranium) and as a result of concerns about proliferation and waste management (e.g. reduced production of plutonium, etc.). Since the average composition of natural Thorium is dominated (100%) by the fertile isotope Th-232, Thorium is only useful as a resource for breeding new fissile materials, in this case U-233. Consequently a certain amount of fissile material must be present at the start-up of the reactor in order to guarantee its operation. The thorium fuel can bemore » used in both once-through and recycle options, and in both fast and thermal spectrum systems. The present study has been aimed by the necessity of investigating the option of using reprocessed plutonium/TRU, from a once-through reference LEU scenario (50 GWd/ tIHM), mixed with natural thorium and the need of collect data (mass fractions, cross-sections etc.) for this particular fuel cycle scenario. As previously pointed out, the fissile plutonium is needed to guarantee the operation of the reactor. Four different scenarios have been considered: • Thorium – recycled Plutonium; • Thorium – recycled Plutonium/Neptunium; • Thorium – recycled Plutonium/Neptunium/Americium; • Thorium – recycled Transuranic. The calculations have been performed with SCALE6.1-TRITON.« less

LWR First Recycle of TRU with Thorium Oxide for Transmutation and Cross Sections

DOE Office of Scientific and Technical Information (OSTI.GOV)

Andrea Alfonsi; Gilles Youinou

2012-07-01

Thorium has been considered as an option to uranium-based fuel, based on considerations of resource utilization (thorium is approximately three times more plentiful than uranium) and as a result of concerns about proliferation and waste management (e.g. reduced production of plutonium, etc.). Since the average composition of natural Thorium is dominated (100%) by the fertile isotope Th-232, Thorium is only useful as a resource for breeding new fissile materials, in this case U-233. Consequently a certain amount of fissile material must be present at the start-up of the reactor in order to guarantee its operation. The thorium fuel can bemore » used in both once-through and recycle options, and in both fast and thermal spectrum systems. The present study has been aimed by the necessity of investigating the option of using reprocessed plutonium/TRU, from a once-through reference LEU scenario (50 GWd/ tIHM), mixed with natural thorium and the need of collect data (mass fractions, cross-sections etc.) for this particular fuel cycle scenario. As previously pointed out, the fissile plutonium is needed to guarantee the operation of the reactor. Four different scenarios have been considered: • Thorium – recycled Plutonium; • Thorium – recycled Plutonium/Neptunium; • Thorium – recycled Plutonium/Neptunium/Americium; • Thorium – recycled Transuranic. The calculations have been performed with SCALE6.1-TRITON.« less

Novel Americium Treatment Process for Surface Water and Dust Suppression Water

DOE Office of Scientific and Technical Information (OSTI.GOV)

Tiepel, E.W.; Pigeon, P.; Nesta, S.

2006-07-01

The Rocky Flats Environmental Technology Site (RFETS), a former nuclear weapons production plant, has been remediated under CERCLA and decommissioned to become a National Wildlife Refuge. The site conducted this cleanup effort under the Rocky Flats Cleanup Agreement (RFCA) that established limits for the discharge of surface and process waters from the site. At the end of 2004, while a number of process buildings were undergoing decommissioning, routine monitoring of a discharge pond (Pond A-4) containing approximately 28 million gallons of water was discovered to have been contaminated with a trace amount of Americium-241 (Am-241). While the amount of Am-241more » in the pond waters was very low (0.5 - 0.7 pCi/l), it was above the established Colorado stream standard of 0.15 pCi/l for release to off site drainage waters. The rapid successful treatment of these waters to the regulatory limit was important to the site for two reasons. The first was that the pond was approaching its hold-up limit. Without rapid treatment and release of the Pond A-4 water, typical spring run-off would require water management actions to other drainages onsite or a mass shuttling of water for disposal. The second reason was that this type of contaminated water had not been treated to the stringent stream standard at Rocky Flats before. Technical challenges in treatment could translate to impacts on water and secondary waste management, and ultimately, cost impacts. All of the technical challenges and specific site criteria led to the conclusion that a different approach to the treatment of this problem was necessary and a crash treatability program to identify applicable treatment techniques was undertaken. The goal of this program was to develop treatment options that could be implemented very quickly and would result in the generation of no high volume secondary waste that would be costly to dispose. A novel chemical treatment system was developed and implemented at the RFETS to treat Am-241 contaminated pond water, surface run-off and D and D dust suppression water during the later stages of the D and D effort at Rocky Flats. This novel chemical treatment system allowed for highly efficient, high-volume treatment of all contaminated waste waters to the very low stream standard of 0.15 pCi/1 with strict compliance to the RFCA discharge criteria for release to off-site surface waters. The rapid development and implementation of the treatment system avoided water management issues that would have had to be addressed if contaminated water had remained in Pond A-4 into the Spring of 2005. Implementation of this treatment system for the Pond A-4 waters and the D and D waters from Buildings 776 and 371 enabled the site to achieve cost-effective treatment that minimized secondary waste generation, avoiding the need for expensive off-site water disposal. Water treatment was conducted for a cost of less than $0.20/gal which included all development costs, capital costs and operational costs. This innovative and rapid response effort saved the RFETS cleanup program well in excess of $30 million for the potential cost of off-site transportation and treatment of radioactive liquid waste. (authors)« less

Light Collection Efficiency in Thin Strip Plastic Scintillator for the Study of ISGMR in Unstable Nuclei

NASA Astrophysics Data System (ADS)

Shafer, Jacob

2011-10-01

The compressibility of nuclear matter (KA) is one of the constituent of the equation of state for nuclear matter which is important in the study Neutron Stars and Super Novae. The KA is proportional to the Giant Monopole Resonance (GMR) energy and is related by the equation EGMR = (h2/mr2) 1/2 *(AKA)1/2 , where ``m'' is the mass of a nucleon and ``r'' is the radius of the nucleus. The GMR in unstable nuclei is important because the KA is related to the ratio of protons to neutrons. For this reason, it is desirable to study unstable nuclei as well as stable nuclei. The study of the GMR in unstable nuclei will be done using inverse kinematics on a target of Lithium (6Li). A detector composed of two layers of thin strip scintillators and one layer of large block scintillators has been designed and constructed to give adequate energy and angular distribution over a large portion of the solid angle where decay particles from the ISGMR can be found. Attenuation of the light signal in the strip scintillators was measured using an Americium (241Am) alpha source. Gains in light collection efficiency due to various wrapping techniques were also measured. The thin strip scintillators are connected to the photomultiplier tube (PMT) via bundles of optical fiber. Losses in light calculation efficiency due to fiber bundles were measured as well. Funded by DOE and NSF-REU.

Electrical Properties of MWCNT/HDPE Composite-Based MSM Structure Under Neutron Irradiation

NASA Astrophysics Data System (ADS)

Kasani, H.; Khodabakhsh, R.; Taghi Ahmadi, M.; Rezaei Ochbelagh, D.; Ismail, Razali

2017-04-01

Because of their low cost, low energy consumption, high performance, and exceptional electrical properties, nanocomposites containing carbon nanotubes are suitable for use in many applications such as sensing systems. In this research work, a metal-semiconductor-metal (MSM) structure based on a multiwall carbon nanotube/high-density polyethylene (MWCNT/HDPE) nanocomposite is introduced as a neutron sensor. Scanning electron microscopy, Fourier-transform infrared, and infrared spectroscopy techniques were used to characterize the morphology and structure of the fabricated device. Current-voltage ( I- V) characteristic modeling showed that the device can be assumed to be a reversed-biased Schottky diode, if the voltage is high enough. To estimate the depletion layer length of the Schottky contact, impedance spectroscopy was employed. Therefore, the real and imaginary parts of the impedance of the MSM system were used to obtain electrical parameters such as the carrier mobility and dielectric constant. Experimental observations of the MSM structure under irradiation from an americium-beryllium (Am-Be) neutron source showed that the current level in the device decreased significantly. Subsequently, current pulses appeared in situ I- V and current-time ( I- t) curve measurements when increasing voltage was applied to the MSM system. The experimentally determined depletion region length as well as the space-charge-limited current mechanism for carrier transport were compared with the range for protons calculated using Monte Carlo n-particle extended (MCNPX) code, yielding the maximum energy of recoiled protons detectable by the device.

Americium-241 and plutonium-237 turnover in mussels ( Mytilus galloprovincialis) living in field enclosures

NASA Astrophysics Data System (ADS)

Guary, J. C.; Fowler, S. W.

1981-02-01

Loss of 241Am and 237Pu from contaminated mussels ( Mytilus galloprovincialis) living in situ in the Mediterranean Sea is described as the sum of three exponential functions. In the case of 241Am, two short-lived compartments representing a total of 80% of the incorporated radionuclide turned over rapidly with biological half-lives of 2 and 3 weeks. The remaining fraction of 241Am, associated with a long-lived compartment, was lost at an extremely slow rate ( Tb1/2=1·3 years). Plutonium-237 turnover in the two short-lived compartments (containing 70% of the Pu) was more rapid ( Tb1/2=1-2 days and 2 weeks) than that of 241Am; however, there was some indication that subsequent loss rates of the two radionuclides in long-lived compartments may be similar if determined over comparable periods of time. Loss rates of 241Am differed for the various tissues, with the most rapid rates occurring in gill, viscera and shell. Abrupt changes in loss observed in muscle and mantle suggested a translocation of 241Am to muscle and mantle during depuration. Whole shell contained by far the largest fraction (˜90%) of both 241Am and 237Pu taken up; in addition, these radionuclides are not irreversibly bound to mussel shell but readily leach into the water. These observations suggest that mollusc shell may influence the biogeochemistry of transuranic elements in littoral zones.

Certification of Plutonium Standards for KAMS Neutron Multiplicity Counter

DOE Office of Scientific and Technical Information (OSTI.GOV)

Salaymeh, S.R.

2002-05-31

As part of the implementation of the PEIS record of decision in January of 1997, DOE will pursue two technologies to disposition fifty metric tons of its stockpile of plutonium. As a result of this and in order to expedite the closure of Rocky Flats Environmental Technology Site in Colorado, DOE decided to use existing facilities at the Savannah River Site (SRS) for storing all material containing plutonium at KAMS. A neutron multiplicity counter was designed and built to carry out receipt verification measurement at the facility. Since the material covers a wide range and different levels of impurities, itmore » is essential that we obtain a set of working standards. An agreement was drafted to select the first drums to be these standards. A plan was developed for the certification of these standards using Rocky Flat's existing nondestructive assay equipment. This paper will discuss the types of materials to be shipped to SRS, number of standards to certify for each type of material, and the certification plan. It will also discuss the activities necessary to determine the nuclear content of these working standards to be used at SRS facilities in support of shipment and receipt of the Pu containing materials. Definition of instrument qualifications, measurement control processes, measurement methodologies, and calculations necessary to report the gram quantities and their uncertainties for plutonium, americium-241, uranium-235 (if present) and neptunium-237 (if present) will also be presented.« less

Self-absorption Effects on Alpha-Induced Atmospheric Nitrogen Fluorescence Yield

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bachelor, Paula P.; Jordan, David V.; Harper, Warren W.

2009-12-01

Nitrogen fluorescence induced by alpha, beta and gamma radiation can be used to detect the presence of radioactive contamination in the environment. Successful measurement of fluorescence yield involves a number of factors, including: known fluorescence signal rate during the measurement; the effective alpha spectrum of the radioactive sources used in the measurement; optical attenuation length of the fluorescence signal in air during the measurement; the absolute throughput of the instrumentation; calibration of the instrumentation; and radiation transport modeling of the "effective" array exposure rate given the spectrum of the alpha particles. Field testing of optical instrumentation was conducted to measuremore » the nitrogen fluorescence yield from the alpha radiation generated from americium-241 (241Am) decay. The 241Am test sources were prepared by direct evaporation of ~1 mCi in nitric acid solution, and some solids were visible on the surface of the sources. A laboratory study was conducted with lower activities of 241Am to determine whether the presence of solids on the surface of the sources prepared both by direct evaporation and by electrodeposition onto stainless steel disks produced sufficient self-absorption to cause a decrease in expected fluorescence. Alpha spectroscopy was used to determine the apparent activity of the sources versus the known activity deposited on the surface. Results from the self-absorption laboratory studies were used to correct the activity values in the model and calculate the nitrogen fluorescence generated by the 241Am during the field experiments.« less

Dirty Bomb Fallout

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gates-Anderson, D; Rasmussen, C; Fischer, R

2007-05-02

At present, there is a significant need to develop decontamination agents that can be used effectively after detonation of a radiological dispersal device (RDD) in an urban environment. There is also a need for the development of reproducible test surfaces to be used to determine the efficacy of the agent being developed. Researchers at Lawrence Livermore National Laboratory (LLNL), under the auspices of the US Department of Energy (DoE), conducted a field study to evaluate the deposition of an explosively dispersed radionuclide surrogate (CsCl) on grime-bearing and non-grime-bearing urban surfaces. The goal was to investigate the preparation and contamination ofmore » urban surfaces that closely mimic what one would expect to encounter following the detonation of an RDD. Migration of Cs into concrete surfaces was investigated in detail. Many non-proliferation, security and response organizations that have modeled RDD scenarios use cesium-137, as well as cobalt-60, strontium-90, americium-241 as the most likely RDD agents. Cesium-137 is an isotope of concern for possible use in an RDD due to its potential availability resulting from its widespread legitimate use in construction, geotechnical and medical industrial devices. In some Cs-containing instruments the Cesium-137 is present as the highly dispersible and water soluble salt, cesium chloride (CsCl). In this form Cs is able to rapidly disperse in the environment, as witnessed in the 1987 Goiania accident in Brazil, when inadvertent dispersal of a radiotherapy source resulted in fatalities and injuries.« less

Electrical characterization of deep levels created by bombarding nitrogen-doped 4H-SiC with alpha-particle irradiation

NASA Astrophysics Data System (ADS)

Omotoso, Ezekiel; Meyer, Walter E.; Auret, F. Danie; Paradzah, Alexander T.; Legodi, Matshisa J.

2016-03-01

Deep-level transient spectroscopy (DLTS) and Laplace-DLTS were used to investigate the effect of alpha-particle irradiation on the electrical properties of nitrogen-doped 4H-SiC. The samples were bombarded with alpha-particles at room temperature (300 K) using an americium-241 (241Am) radionuclide source. DLTS revealed the presence of four deep levels in the as-grown samples, E0.09, E0.11, E0.16 and E0.65. After irradiation with a fluence of 4.1 × 1010 alpha-particles-cm-2, DLTS measurements indicated the presence of two new deep levels, E0.39 and E0.62 with energy levels, EC - 0.39 eV and EC - 0.62 eV, with an apparent capture cross sections of 2 × 10-16 and 2 × 10-14 cm2, respectively. Furthermore, irradiation with fluence of 8.9 × 1010 alpha-particles-cm-2 resulted in the disappearance of shallow defects due to a lowering of the Fermi level. These defects re-appeared after annealing at 300 °C for 20 min. Defects, E0.39 and E0.42 with close emission rates were attributed to silicon or carbon vacancy and could only be separated by using high resolution Laplace-DLTS. The DLTS peaks at EC - (0.55-0.70) eV (known as Z1/Z2) were attributed to an isolated carbon vacancy (VC).

A Monte Carlo Simulation of the in vivo measurement of lung activity in the Lawrence Livermore National Laboratory torso phantom.

PubMed

Acha, Robert; Brey, Richard; Capello, Kevin

2013-02-01

A torso phantom was developed by the Lawrence Livermore National Laboratory (LLNL) that serves as a standard for intercomparison and intercalibration of detector systems used to measure low-energy photons from radionuclides, such as americium deposited in the lungs. DICOM images of the second-generation Human Monitoring Laboratory-Lawrence Livermore National Laboratory (HML-LLNL) torso phantom were segmented and converted into three-dimensional (3D) voxel phantoms to simulate the response of high purity germanium (HPGe) detector systems, as found in the HML new lung counter using a Monte Carlo technique. The photon energies of interest in this study were 17.5, 26.4, 45.4, 59.5, 122, 244, and 344 keV. The detection efficiencies at these photon energies were predicted for different chest wall thicknesses (1.49 to 6.35 cm) and compared to measured values obtained with lungs containing (241)Am (34.8 kBq) and (152)Eu (10.4 kBq). It was observed that no statistically significant differences exist at the 95% confidence level between the mean values of simulated and measured detection efficiencies. Comparisons between the simulated and measured detection efficiencies reveal a variation of 20% at 17.5 keV and 1% at 59.5 keV. It was found that small changes in the formulation of the tissue substitute material caused no significant change in the outcome of Monte Carlo simulations.

Trends in the short-term release of fission products and actinides to aqueous solution from used CANDU fuels at elevated temperature

NASA Astrophysics Data System (ADS)

Stroes-Gascoyne, S.

1992-08-01

A large number of short-term leaching experiments has been performed to determine fission product and actinide release from used CANDU (CANada Deuterium Uranium) fuels and to establish which factors affect release. Results are reported after30 ± 10 d leaching at 100-150°C under oxidizing (air) or reducing (Ar-3% H 2 or Ar) conditions, in various synthetic groundwaters. Cesium-137 release (0.007-6%) was positively correlated with increases in fuel power, leachant temperature and ionic strength. Strontium-90 release (0.0003-0.3%) generally increased with ionic strength, higher temperature and redox conditions. Actinide and Tc concentrations were compared to ranges calculated with a thermodynamic equilibrium model, that accounts for the uncertain geochemical parameters of a nuclear waste vault by calculating concentration ranges based on 40000 hypothetical cases. Experimental U concentrations (10 -8.5 to 10 -3 mol/kg) were higher than the model range, probably because of higher redox potentials in the experiments. Measured Pu concentrations (10 -12.5 to 10 -7 mol/kg) were at the low end of the calculated range. Americium and Cm concentrations (10 -12.5 to 10 -7 and 10 -15 to 10 -9 mol/kg, respectively) were highest under oxidizing conditions and higher temperatures. Technetium-99 concentrations (10 -5.5 to 10 -10.5 mol/kg) covered a much narrower range than calculated by the model.

Modelling the behaviour of oxide fuels containing minor actinides with urania, thoria and zirconia matrices in an accelerator-driven system

NASA Astrophysics Data System (ADS)

Sobolev, V.; Lemehov, S.; Messaoudi, N.; Van Uffelen, P.; Aı̈t Abderrahim, H.

2003-06-01

The Belgian Nuclear Research Centre, SCK • CEN, is currently working on the pre-design of the multipurpose accelerator-driven system (ADS) MYRRHA. A demonstration of the possibility of transmutation of minor actinides and long-lived fission products with a realistic design of experimental fuel targets and prognosis of their behaviour under typical ADS conditions is an important task in the MYRRHA project. In the present article, the irradiation behaviour of three different oxide fuel mixtures, containing americium and plutonium - (Am,Pu,U)O 2- x with urania matrix, (Am,Pu,Th)O 2- x with thoria matrix and (Am,Y,Pu,Zr)O 2- x with inert zirconia matrix stabilised by yttria - were simulated with the new fuel performance code MACROS, which is under development and testing at the SCK • CEN. All the fuel rods were considered to be of the same design and sizes: annular fuel pellets, helium bounded with the stainless steel cladding, and a large gas plenum. The liquid lead-bismuth eutectic was used as coolant. Typical irradiation conditions of the hottest fuel assembly of the MYRRHA subcritical core were pre-calculated with the MCNPX code and used in the following calculations as the input data. The results of prediction of the thermo-mechanical behaviour of the designed rods with the considered fuels during three irradiation cycles of 90 EFPD are presented and discussed.

Characterization of Uranium Contamination, Transport, and Remediation at Rocky Flats - Across Remediation into Post-Closure

NASA Astrophysics Data System (ADS)

Janecky, D. R.; Boylan, J.; Murrell, M. T.

2009-12-01

The Rocky Flats Site is a former nuclear weapons production facility approximately 16 miles northwest of Denver, Colorado. Built in 1952 and operated by the Atomic Energy Commission and then Department of Energy, the Site was remediated and closed in 2005, and is currently undergoing long-term surveillance and monitoring by the DOE Office of Legacy Management. Areas of contamination resulted from roughly fifty years of operation. Of greatest interest, surface soils were contaminated with plutonium, americium, and uranium; groundwater was contaminated with chlorinated solvents, uranium, and nitrates; and surface waters, as recipients of runoff and shallow groundwater discharge, have been contaminated by transport from both regimes. A region of economic mineralization that has been referred to as the Colorado Mineral Belt is nearby, and the Schwartzwalder uranium mine is approximately five miles upgradient of the Site. Background uranium concentrations are therefore elevated in many areas. Weapons-related activities included work with enriched and depleted uranium, contributing anthropogenic content to the environment. Using high-resolution isotopic analyses, Site-related contamination can be distinguished from natural uranium in water samples. This has been instrumental in defining remedy components, and long-term monitoring and surveillance strategies. Rocky Flats hydrology interlinks surface waters and shallow groundwater (which is very limited in volume and vertical and horizontal extent). Surface water transport pathways include several streams, constructed ponds, and facility surfaces. Shallow groundwater has no demonstrated connection to deep aquifers, and includes natural preferential pathways resulting primarily from porosity in the Rocky Flats alluvium, weathered bedrock, and discontinuous sandstones. In addition, building footings, drains, trenches, and remedial systems provide pathways for transport at the site. Removal of impermeable surfaces (buildings, roads, and so on) during the Site closure efforts resulted in major changes to surface and shallow groundwater flow. Consistent with previous documentation of uranium operations and contamination, only very small amounts of highly enriched uranium are found in a small number of water samples, generally from the former Solar Ponds complex and central Industrial Area. Depleted uranium is more widely distributed at the site, and water samples exhibit the full range of depleted plus natural uranium mixtures. However, one third of the samples are found to contain only natural uranium, and three quarters of the samples are found to contain more than 90% natural uranium - substantial fractions given that the focus of these analyses was on evaluating potentially contaminated waters. Following site closure, uranium concentrations have increased at some locations, particularly for surface water samples. Overall, isotopic ratios at individual locations have been relatively consistent, indicating that the increases in concentrations are due to decreases in dilution flow following removal of impermeable surfaces and buildings.

Beryllium-7 and lead-210 chronometry of modern soil processes: The Linked Radionuclide aCcumulation model, LRC

NASA Astrophysics Data System (ADS)

Landis, Joshua D.; Renshaw, Carl E.; Kaste, James M.

2016-05-01

Soil systems are known to be repositories for atmospheric carbon and metal contaminants, but the complex processes that regulate the introduction, migration and fate of atmospheric elements in soils are poorly understood. This gap in knowledge is attributable, in part, to the lack of an established chronometer that is required for quantifying rates of relevant processes. Here we develop and test a framework for adapting atmospheric lead-210 chronometry (210Pb; half-life 22 years) to soil systems. We propose a new empirical model, the Linked Radionuclide aCcumulation model (LRC, aka "lark"), that incorporates measurements of beryllium-7 (7Be; half-life 54 days) to account for 210Pb penetration of the soil surface during initial deposition, a process which is endemic to soils but omitted from conventional 210Pb models (e.g., the Constant Rate of Supply, CRS model) and their application to sedimentary systems. We validate the LRC model using the 1963-1964 peak in bomb-fallout americium-241 (241Am; half-life of 432 years) as an independent, corroborating time marker. In three different soils we locate a sharp 241Am weapons horizon at disparate depths ranging from 2.5 to 6 cm, but with concordant ages averaging 1967 ± 4 via the LRC model. Similarly, at one site contaminated with mercury (HgT) we find that the LRC model is consistent with the recorded history of Hg emission. The close agreement of Pb, Am and Hg behavior demonstrated here suggests that organo-metallic colloid formation and migration incorporates many trace metals in universal soil processes and that these processes may be described quantitatively using atmospheric 210Pb chronometry. The 210Pb models evaluated here show that migration rates of soil colloids on the order of 1 mm yr-1 are typical, but also that these rates vary systematically with depth and are attributable to horizon-specific processes of leaf-litter decay, eluviation and illuviation. We thus interpret 210Pb models to quantify (i) exposure of the soil system to atmospheric aerosol deposition in the context of (ii) organic carbon assimilation, colloid production, and advection through the soil profile. The behavior of some other elements, such as Cs, diverges from the conservative colloid behavior exemplified by Pb and Am, and in these cases the value of empirical 210Pb chronometry models like LRC and CRS is as a comparator rather than as an absolute chronometer. We conclude that 210Pb chronometry is valuable for tracing colloidally-mediated transport of Pb and similarly-refractory metals, as well as the mobile pool of carbon in soils.

Uncovering the Origin of Divergence in the CsM(CrO 4) 2 (M = La, Pr, Nd, Sm, Eu; Am) Family through Examination of the Chemical Bonding in a Molecular Cluster and by Band Structure Analysis

DOE Office of Scientific and Technical Information (OSTI.GOV)

Galley, Shane S.; Arico, Alexandra A.; Lee, Tsung-Han

A series of f-block chromates, CsM(CrO 4) 2 (M = La, Pr, Nd, Sm, Eu; Am), were prepared revealing notable differences between the Am III derivatives and their lanthanide analogs. While all compounds form similar layered structures, the americium compound exhibits polymorphism and adopts both a structure isomorphous with the early lanthanides as well as one that possesses lower symmetry. Both polymorphs are dark red and possess band gaps that are smaller than the Ln III compounds. In order to probe the origin of these differences, the electronic structure of α-CsSm(CrO 4) 2, α-CsEu(CrO 4) 2, and α-CsAm(CrO 4) 2more » were studied using both a molecular cluster approach featuring hybrid density functional theory and QTAIM analysis and by the periodic LDA+GA and LDA+DMFT methods. Notably, the covalent contributions to bonding by the f orbitals were found to be more than twice as large in the Am III chromate than in the Sm III and Eu III compounds, and even larger in magnitude than the Am-5f spin–orbit splitting in this system. Our analysis indicates also that the Am–O covalency in α-CsAm(CrO 4) 2 is driven by the degeneracy of the 5f and 2p orbitals, and not by orbital overlap.« less

Background Radioactivity in River and Reservoir Sediments near Los Alamos, New Mexico

DOE Office of Scientific and Technical Information (OSTI.GOV)

S.G.McLin; D.W. Lyons

2002-05-05

As part of its continuing Environmental Surveillance Program, regional river and lake-bottom sediments have been collected annually by Los Alamos National Laboratory (the Laboratory) since 1974 and 1979, respectively. These background samples are collected from three drainage basins at ten different river stations and five reservoirs located throughout northern New Mexico and southern Colorado. Radiochemical analyses for these sediments include tritium, strontium-90, cesium-137, total uranium, plutonium-238, plutonium-239,-240, americium-241, gross alpha, gross beta, and gross gamma radioactivity. Detection-limit radioactivity originates as worldwide fallout from aboveground nuclear weapons testing and satellite reentry into Earth's atmosphere. Spatial and temporal variations in individual analytemore » levels originate from atmospheric point-source introductions and natural rate differences in airborne deposition and soil erosion. Background radioactivity values on sediments reflect this variability, and grouped river and reservoir sediment samples show a range of statistical distributions that appear to be analyte dependent. Traditionally, both river and reservoir analyte data were blended together to establish background levels. In this report, however, we group background sediment data according to two criteria. These include sediment source (either river or reservoir sediments) and station location relative to the Laboratory (either upstream or downstream). These grouped data are statistically evaluated through 1997, and background radioactivity values are established for individual analytes in upstream river and reservoir sediments. This information may be used to establish the existence and areal extent of trace-level environmental contamination resulting from historical Laboratory research activities since the early 1940s.« less

Uncovering the Origin of Divergence in the CsM(CrO 4) 2 (M = La, Pr, Nd, Sm, Eu; Am) Family through Examination of the Chemical Bonding in a Molecular Cluster and by Band Structure Analysis

DOE PAGES

Galley, Shane S.; Arico, Alexandra A.; Lee, Tsung-Han; ...

2018-01-10

A series of f-block chromates, CsM(CrO 4) 2 (M = La, Pr, Nd, Sm, Eu; Am), were prepared revealing notable differences between the Am III derivatives and their lanthanide analogs. While all compounds form similar layered structures, the americium compound exhibits polymorphism and adopts both a structure isomorphous with the early lanthanides as well as one that possesses lower symmetry. Both polymorphs are dark red and possess band gaps that are smaller than the Ln III compounds. In order to probe the origin of these differences, the electronic structure of α-CsSm(CrO 4) 2, α-CsEu(CrO 4) 2, and α-CsAm(CrO 4) 2more » were studied using both a molecular cluster approach featuring hybrid density functional theory and QTAIM analysis and by the periodic LDA+GA and LDA+DMFT methods. Notably, the covalent contributions to bonding by the f orbitals were found to be more than twice as large in the Am III chromate than in the Sm III and Eu III compounds, and even larger in magnitude than the Am-5f spin–orbit splitting in this system. Our analysis indicates also that the Am–O covalency in α-CsAm(CrO 4) 2 is driven by the degeneracy of the 5f and 2p orbitals, and not by orbital overlap.« less

An initial demonstration of hierarchically porous niobium alkylphosphonates coordination polymers as potent radioanalytical separation materials.

PubMed

Lv, Kai; Yang, Chu-Ting; Han, Jun; Hu, Sheng; Wang, Xiao-Lin

2017-06-30

Combining the merits of soft-templating and perchlorate oxidation methods, the first-case investigation of niobium alkylphosphonates has uncovered their unique morphology, backbone composition, thermal behavior and huge potentiality as radioanalytical separation materials. These hierarchically porous solids are random aggregates of densely stacked nanolayers perforated with worm-like holes or vesicular voids, manifesting the massif-, tower-like "polymer brush" elevated up to ∼150nm driven by the minimal surface free energy principle. These coordination polymers consist of distorted niobium (V) ions strongly linked with tetrahedral alkylphosphonate building units, exposing uncoordinated phosphonate moieties and defective metal sites. Despite the amorphous features, they demonstrate multimodal porosity covering continuous micropores, segregated mesopores and fractional macropores, beneficial for the sequestration by active Lewis acid-base center. Evidenced by the maximum distribution coefficients of thorium, lanthanides reaching 9.0×10 4 , 9.5×10 4 mLg -1 and large separation factor at pH≤1 20-element cocktail, this category of niobium alkylphosphonates are capable of harvesting thorium, lanthanides directly from the radionuclide surrogate, comparable to or even surpass the performance of the metal (IV) arylphosphonates counterparts. They also display appreciable SF Eu/Sm ∼20 in 1molL -1 HNO 3 , shedding light on dual approaches to achieve the isolation of americium from curium. A combinatorial radioanalytical separation protocol has been proposed to enrich thorium and europium, revealing facile utilization of these highly stable, phosphonated hybrids in sustainable development of radioanalytical separation. Copyright © 2017 Elsevier B.V. All rights reserved.

Effect of Potassium on Uptake of 137Cs in Food Crops Grown on Coral Soils: Annual Crops at Bikini Atoll

DOE Office of Scientific and Technical Information (OSTI.GOV)

Stone, E R; Robinson, W

2002-02-01

In 1954 a radioactive plume from the thermonuclear device code named BRAVO contaminated the principal residential islands, Eneu and Bikini, of Bikini Atoll (11{sup o} 36 minutes N; 165{sup o} 22 minutes E), now part of the Republic of the Marshall Islands. The resulting soil radioactivity diminished greatly over the three decades before the studies discussed below began. By that time the shorter-lived isotopes had all but disappeared, but strontium-90 ({sup 90}Sr), and cesium-137, ({sup 137}Cs) were reduced by only one half-life. Minute amounts of the long-lived isotopes, plutonium-239+240 ({sup 239+240}Pu) and americium-241 ({sup 241}Am), were present in soil, butmore » were found to be inconsequential in the food chain of humans and land animals. Rather, extensive studies demonstrated that the major concern for human health was {sup 137}Cs in the terrestrial food chain (Robison et al., 1983; Robison et al., 1997). The following papers document results from several studies between 1986 and 1997 aimed at minimizing the {sup 137}Cs content of annual food crops. The existing literature on radiocesium in soils and plant uptake is largely a consequence of two events: the worldwide fallout of 1952-58, and the fallout from Chernobyl. The resulting studies have, for the most part, dealt either with soils containing some amount of silicate clays and often with appreciable K, or with the short-term development of plants in nutrient cultures.« less